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</div> <div class="control"> <button class="button is-small is-link">Go</button> </div> </div> </form> </div> </div> <nav class="pagination is-small is-centered breathe-horizontal" role="navigation" aria-label="pagination"> <a href="" class="pagination-previous is-invisible">Previous </a> <a href="/search/?searchtype=author&query=Bucksbaum%2C+P+H&start=50" class="pagination-next" >Next </a> <ul class="pagination-list"> <li> <a href="/search/?searchtype=author&query=Bucksbaum%2C+P+H&start=0" class="pagination-link is-current" aria-label="Goto page 1">1 </a> </li> <li> <a href="/search/?searchtype=author&query=Bucksbaum%2C+P+H&start=50" class="pagination-link " aria-label="Page 2" aria-current="page">2 </a> </li> </ul> </nav> <ol class="breathe-horizontal" start="1"> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2411.04144">arXiv:2411.04144</a> <span> [<a href="https://arxiv.org/pdf/2411.04144">pdf</a>, <a href="https://arxiv.org/format/2411.04144">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> </div> <p class="title is-5 mathjax"> Orientation-Dependent Enhanced Ionization in Acetylene Revealed by Ultrafast Cross-Polarized Pulse Pairs </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Mohideen%2C+S+A">S. A. Mohideen</a>, <a href="/search/physics?searchtype=author&query=Howard%2C+A+J">A. J. Howard</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+C">C. Cheng</a>, <a href="/search/physics?searchtype=author&query=Gabalski%2C+I">I. Gabalski</a>, <a href="/search/physics?searchtype=author&query=Ghrist%2C+A+M">A. M. Ghrist</a>, <a href="/search/physics?searchtype=author&query=Weckwerth%2C+E">E. Weckwerth</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2411.04144v1-abstract-short" style="display: inline;"> We investigate the orientation dependence of Enhanced Ionization (EI) during strong-field-driven nuclear motion in acetylene (C$_2$H$_2$). Here, we both initiate and probe molecular dynamics in acetylene with intense 6-fs cross-polarized pulse pairs, separated by a variable delay. Following multiple ionization by the first pulse, acetylene undergoes simultaneous elongation of the carbon-carbon and… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2411.04144v1-abstract-full').style.display = 'inline'; document.getElementById('2411.04144v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2411.04144v1-abstract-full" style="display: none;"> We investigate the orientation dependence of Enhanced Ionization (EI) during strong-field-driven nuclear motion in acetylene (C$_2$H$_2$). Here, we both initiate and probe molecular dynamics in acetylene with intense 6-fs cross-polarized pulse pairs, separated by a variable delay. Following multiple ionization by the first pulse, acetylene undergoes simultaneous elongation of the carbon-carbon and carbon-hydrogen bonds, enabling further ionization by the second pulse and the formation of a very highly charged state, [C$_2$H$_2]^{6+}$. At small inter-pulse delays ($<$20 fs), this enhancement occurs when the molecule is aligned to the probe pulse. Conversely, at large delays ($>$40 fs), formation of [C$_2$H$_2]^{6+}$ occurs when the molecule is aligned to the pump pulse. By analyzing the polarization and time dependence of sequentially ionized [C$_2$H$_2]^{6+}$, we resolve two distinct pathways that both contribute to a large increase in the multiple ionization yield. This cross-polarized pulse pair scheme uniquely enables selective probing of deeply bound orbitals, providing new insights on orientation-dependent EI in highly charged hydrocarbons. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2411.04144v1-abstract-full').style.display = 'none'; document.getElementById('2411.04144v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 5 November, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> November 2024. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2411.01729">arXiv:2411.01729</a> <span> [<a href="https://arxiv.org/pdf/2411.01729">pdf</a>, <a href="https://arxiv.org/format/2411.01729">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Data Analysis, Statistics and Probability">physics.data-an</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> </div> <p class="title is-5 mathjax"> Covariance Analysis of Impulsive Streaking </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Wang%2C+J">Jun Wang</a>, <a href="/search/physics?searchtype=author&query=Guo%2C+Z">Zhaoheng Guo</a>, <a href="/search/physics?searchtype=author&query=Isele%2C+E">Erik Isele</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Marinelli%2C+A">Agostino Marinelli</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2411.01729v1-abstract-short" style="display: inline;"> A comprehensive framework of modeling covariance in angular streaking experiments is presented. Within the impulsive streaking regime, the displacement of electron momentum distribution (MD) provides a tight connection between the dressing-free MD and the dressed MD. Such connection establishes universal structures in the composition of streaking covariance that are common across different MDs, re… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2411.01729v1-abstract-full').style.display = 'inline'; document.getElementById('2411.01729v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2411.01729v1-abstract-full" style="display: none;"> A comprehensive framework of modeling covariance in angular streaking experiments is presented. Within the impulsive streaking regime, the displacement of electron momentum distribution (MD) provides a tight connection between the dressing-free MD and the dressed MD. Such connection establishes universal structures in the composition of streaking covariance that are common across different MDs, regardless of their exact shape. Building on this robust framework, we have developed methods for retrieving temporal information from angular streaking measurements. By providing a detailed understanding of the covariance structure in angular streaking experiments, our work enables more accurate and robust temporal measurements in a wide range of experimental scenarios. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2411.01729v1-abstract-full').style.display = 'none'; document.getElementById('2411.01729v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 3 November, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> November 2024. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">22 pages, 13 figures</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2411.01700">arXiv:2411.01700</a> <span> [<a href="https://arxiv.org/pdf/2411.01700">pdf</a>, <a href="https://arxiv.org/format/2411.01700">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> </div> <p class="title is-5 mathjax"> Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a>, <a href="/search/physics?searchtype=author&query=Guo%2C+Z">Zhaoheng Guo</a>, <a href="/search/physics?searchtype=author&query=Isele%2C+E">Erik Isele</a>, <a href="/search/physics?searchtype=author&query=Grell%2C+G">Gilbert Grell</a>, <a href="/search/physics?searchtype=author&query=Ruberti%2C+M">Marco Ruberti</a>, <a href="/search/physics?searchtype=author&query=ONeal%2C+J+T">Jordan T. ONeal</a>, <a href="/search/physics?searchtype=author&query=Alexander%2C+O">Oliver Alexander</a>, <a href="/search/physics?searchtype=author&query=Beauvarlet%2C+S">Sandra Beauvarlet</a>, <a href="/search/physics?searchtype=author&query=Cesar%2C+D">David Cesar</a>, <a href="/search/physics?searchtype=author&query=Duris%2C+J">Joseph Duris</a>, <a href="/search/physics?searchtype=author&query=Garratt%2C+D">Douglas Garratt</a>, <a href="/search/physics?searchtype=author&query=Larsen%2C+K+A">Kirk A. Larsen</a>, <a href="/search/physics?searchtype=author&query=Li%2C+S">Siqi Li</a>, <a href="/search/physics?searchtype=author&query=Koloren%C4%8D%2C+P">P艡emysl Koloren膷</a>, <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">Gregory A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Tuthill%2C+D">Daniel Tuthill</a>, <a href="/search/physics?searchtype=author&query=Wang%2C+Z">Zifan Wang</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">Nora Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">Christoph Bostedt</a>, <a href="/search/physics?searchtype=author&query=Borne%2C+K">Kurtis Borne</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+X">Xinxin Cheng</a>, <a href="/search/physics?searchtype=author&query=DiMauro%2C+L+F">Louis F. DiMauro</a>, <a href="/search/physics?searchtype=author&query=Doumy%2C+G">Gilles Doumy</a>, <a href="/search/physics?searchtype=author&query=Franz%2C+P+L">Paris L. Franz</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a> , et al. (28 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2411.01700v1-abstract-short" style="display: inline;"> In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this work, we employ a pair of attosecond x-ray pulses from an x-ray free-electron laser to follow electron motion resulting from the sudden removal of an electron from… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2411.01700v1-abstract-full').style.display = 'inline'; document.getElementById('2411.01700v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2411.01700v1-abstract-full" style="display: none;"> In molecular systems, the ultrafast motion of electrons initiates the process of chemical change. Tracking this electronic motion across molecules requires coupling attosecond time resolution to atomic-scale spatial sensitivity. In this work, we employ a pair of attosecond x-ray pulses from an x-ray free-electron laser to follow electron motion resulting from the sudden removal of an electron from a prototypical aromatic system, para-aminophenol. X-ray absorption enables tracking this motion with atomic-site specificity. Our measurements are compared with state-of-the-art computational modeling, reproducing the observed response across multiple timescales. Sub-femtosecond dynamics are assigned to states undergoing non-radiative decay, while few-femtosecond oscillatory motion is associated with electronic wavepacket motion in stable cation states, that will eventually couple to nuclear motion. Our work provides insight on the ultrafast charge motion preceding and initiating chemical transformations in moderately complex systems, and provides a powerful benchmark for computational models of ultrafast charge motion in matter. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2411.01700v1-abstract-full').style.display = 'none'; document.getElementById('2411.01700v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 3 November, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> November 2024. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2408.09056">arXiv:2408.09056</a> <span> [<a href="https://arxiv.org/pdf/2408.09056">pdf</a>, <a href="https://arxiv.org/format/2408.09056">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> </div> <p class="title is-5 mathjax"> Isotope-Selective Strong Field Ionization of Semi-Heavy Water </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Howard%2C+A+J">Andrew J. Howard</a>, <a href="/search/physics?searchtype=author&query=Britton%2C+M">M. Britton</a>, <a href="/search/physics?searchtype=author&query=Streeter%2C+Z+L">Zachary L. Streeter</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+C">Chuan Cheng</a>, <a href="/search/physics?searchtype=author&query=Lucchese%2C+R+R">Robert R. Lucchese</a>, <a href="/search/physics?searchtype=author&query=McCurdy%2C+C+W">C. William McCurdy</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2408.09056v1-abstract-short" style="display: inline;"> Semi-heavy water (HOD) is one of the simplest molecules in which the bonds are labelled by isotope. We demonstrate that a pair of intense few-femtosecond infrared laser pulses can be used to selectively tunnel ionize along one of the two bonds. The first pulse doubly ionizes HOD, inducing rapid bond stretching and unbending. Femtoseconds later, the second pulse arrives and further ionization is se… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2408.09056v1-abstract-full').style.display = 'inline'; document.getElementById('2408.09056v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2408.09056v1-abstract-full" style="display: none;"> Semi-heavy water (HOD) is one of the simplest molecules in which the bonds are labelled by isotope. We demonstrate that a pair of intense few-femtosecond infrared laser pulses can be used to selectively tunnel ionize along one of the two bonds. The first pulse doubly ionizes HOD, inducing rapid bond stretching and unbending. Femtoseconds later, the second pulse arrives and further ionization is selectively enhanced along the OH bond. These conclusions arise from 3D time-resolved measurements of H$^+$, D$^+$, and O$^+$ momenta following triple ionization. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2408.09056v1-abstract-full').style.display = 'none'; document.getElementById('2408.09056v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 16 August, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> August 2024. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">Supplemental Materials included at the end of the main text</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2406.13083">arXiv:2406.13083</a> <span> [<a href="https://arxiv.org/pdf/2406.13083">pdf</a>, <a href="https://arxiv.org/format/2406.13083">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Instrumentation and Detectors">physics.ins-det</span> </div> </div> <p class="title is-5 mathjax"> Design and Performance of a Magnetic Bottle Electron Spectrometer for High-Energy Photoelectron Spectroscopy </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Borne%2C+K">Kurtis Borne</a>, <a href="/search/physics?searchtype=author&query=ONeal%2C+J+T">Jordan T ONeal</a>, <a href="/search/physics?searchtype=author&query=Wang%2C+J">Jun Wang</a>, <a href="/search/physics?searchtype=author&query=Isele%2C+E">Erk Isele</a>, <a href="/search/physics?searchtype=author&query=Obaid%2C+R">Razib Obaid</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">Nora Berrah</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+X">Xinxin Cheng</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=James%2C+J">Justin James</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andri Kamalov</a>, <a href="/search/physics?searchtype=author&query=Larsen%2C+K+A">Kirk A Larsen</a>, <a href="/search/physics?searchtype=author&query=Li%2C+X">Xiang Li</a>, <a href="/search/physics?searchtype=author&query=Lin%2C+M">Ming-Fu Lin</a>, <a href="/search/physics?searchtype=author&query=Liu%2C+Y">Yusong Liu</a>, <a href="/search/physics?searchtype=author&query=Marinelli%2C+A">Agostino Marinelli</a>, <a href="/search/physics?searchtype=author&query=Summers%2C+A">Adam Summers</a>, <a href="/search/physics?searchtype=author&query=Thierstein%2C+E">Emily Thierstein</a>, <a href="/search/physics?searchtype=author&query=Wolf%2C+T">Thomas Wolf</a>, <a href="/search/physics?searchtype=author&query=Rolles%2C+D">Daniel Rolles</a>, <a href="/search/physics?searchtype=author&query=Walter%2C+P">Peter Walter</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P Cryan</a>, <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2406.13083v2-abstract-short" style="display: inline;"> We describe the design and performance of a magnetic bottle electron spectrometer~(MBES) for high-energy electron spectroscopy. Our design features a ${\sim2}$~m long electron drift tube and electrostatic retardation lens, achieving sub-electronvolt (eV) electron kinetic energy resolution for high energy (several hundred eV) electrons with close to 4$蟺$ collection efficiency. A segmented anode… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2406.13083v2-abstract-full').style.display = 'inline'; document.getElementById('2406.13083v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2406.13083v2-abstract-full" style="display: none;"> We describe the design and performance of a magnetic bottle electron spectrometer~(MBES) for high-energy electron spectroscopy. Our design features a ${\sim2}$~m long electron drift tube and electrostatic retardation lens, achieving sub-electronvolt (eV) electron kinetic energy resolution for high energy (several hundred eV) electrons with close to 4$蟺$ collection efficiency. A segmented anode electron detector enables the simultaneous collection of photoelectron spectra in high resolution and high collection efficiency modes. This versatile instrument is installed at the TMO endstation at the LCLS x-ray free-electron laser (XFEL). In this paper, we demonstrate its high resolution, collection efficiency and spatial selectivity in measurements where it is coupled to an XFEL source. These combined characteristics are designed to enable high-resolution time-resolved measurements using x-ray photoelectron, absorption, and Auger-Meitner spectroscopy. We also describe the pervasive artifact in MBES time-of-flight spectra that arises from a periodic modulation in electron detection efficiency, and present a robust analysis procedure for its removal. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2406.13083v2-abstract-full').style.display = 'none'; document.getElementById('2406.13083v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 4 July, 2024; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 18 June, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> June 2024. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2402.12764">arXiv:2402.12764</a> <span> [<a href="https://arxiv.org/pdf/2402.12764">pdf</a>, <a href="https://arxiv.org/format/2402.12764">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> </div> <p class="title is-5 mathjax"> Attosecond Delays in X-ray Molecular Ionization </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a>, <a href="/search/physics?searchtype=author&query=Mountney%2C+M">Miles Mountney</a>, <a href="/search/physics?searchtype=author&query=Wang%2C+J">Jun Wang</a>, <a href="/search/physics?searchtype=author&query=Ortmann%2C+L">Lisa Ortmann</a>, <a href="/search/physics?searchtype=author&query=Al-Haddad%2C+A">Andre Al-Haddad</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">Nora Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">Christoph Bostedt</a>, <a href="/search/physics?searchtype=author&query=Champenois%2C+E+G">Elio G. Champenois</a>, <a href="/search/physics?searchtype=author&query=DiMauro%2C+L+F">Louis F. DiMauro</a>, <a href="/search/physics?searchtype=author&query=Duris%2C+J">Joseph Duris</a>, <a href="/search/physics?searchtype=author&query=Garratt%2C+D">Douglas Garratt</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">James M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Guo%2C+Z">Zhaoheng Guo</a>, <a href="/search/physics?searchtype=author&query=Haxton%2C+D">Daniel Haxton</a>, <a href="/search/physics?searchtype=author&query=Isele%2C+E">Erik Isele</a>, <a href="/search/physics?searchtype=author&query=Ivanov%2C+I">Igor Ivanov</a>, <a href="/search/physics?searchtype=author&query=Ji%2C+J">Jiabao Ji</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a>, <a href="/search/physics?searchtype=author&query=Li%2C+S">Siqi Li</a>, <a href="/search/physics?searchtype=author&query=Lin%2C+M">Ming-Fu Lin</a>, <a href="/search/physics?searchtype=author&query=Marangos%2C+J+P">Jon P. Marangos</a>, <a href="/search/physics?searchtype=author&query=Obaid%2C+R">Razib Obaid</a>, <a href="/search/physics?searchtype=author&query=O%27Neal%2C+J+T">Jordan T. O'Neal</a>, <a href="/search/physics?searchtype=author&query=Rosenberger%2C+P">Philipp Rosenberger</a>, <a href="/search/physics?searchtype=author&query=Shivaram%2C+N+H">Niranjan H. Shivaram</a> , et al. (12 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2402.12764v1-abstract-short" style="display: inline;"> The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) phot… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2402.12764v1-abstract-full').style.display = 'inline'; document.getElementById('2402.12764v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2402.12764v1-abstract-full" style="display: none;"> The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. The results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2402.12764v1-abstract-full').style.display = 'none'; document.getElementById('2402.12764v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 20 February, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> February 2024. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2401.15250">arXiv:2401.15250</a> <span> [<a href="https://arxiv.org/pdf/2401.15250">pdf</a>, <a href="https://arxiv.org/format/2401.15250">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Accelerator Physics">physics.acc-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> </div> <p class="title is-5 mathjax"> Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Guo%2C+Z">Zhaoheng Guo</a>, <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a>, <a href="/search/physics?searchtype=author&query=Beauvarlet%2C+S">Sandra Beauvarlet</a>, <a href="/search/physics?searchtype=author&query=Cesar%2C+D">David Cesar</a>, <a href="/search/physics?searchtype=author&query=Duris%2C+J">Joseph Duris</a>, <a href="/search/physics?searchtype=author&query=Franz%2C+P+L">Paris L. Franz</a>, <a href="/search/physics?searchtype=author&query=Alexander%2C+O">Oliver Alexander</a>, <a href="/search/physics?searchtype=author&query=Bohler%2C+D">Dorian Bohler</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">Christoph Bostedt</a>, <a href="/search/physics?searchtype=author&query=Averbukh%2C+V">Vitali Averbukh</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+X">Xinxin Cheng</a>, <a href="/search/physics?searchtype=author&query=DiMauro%2C+L+F">Louis F. DiMauro</a>, <a href="/search/physics?searchtype=author&query=Doumy%2C+G">Gilles Doumy</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">Ruaridh Forbes</a>, <a href="/search/physics?searchtype=author&query=Gessner%2C+O">Oliver Gessner</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">James M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Isele%2C+E">Erik Isele</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a>, <a href="/search/physics?searchtype=author&query=Larsen%2C+K+A">Kirk A. Larsen</a>, <a href="/search/physics?searchtype=author&query=Li%2C+S">Siqi Li</a>, <a href="/search/physics?searchtype=author&query=Li%2C+X">Xiang Li</a>, <a href="/search/physics?searchtype=author&query=Lin%2C+M">Ming-Fu Lin</a>, <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">Gregory A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Obaid%2C+R">Razib Obaid</a>, <a href="/search/physics?searchtype=author&query=ONeal%2C+J+T">Jordan T. ONeal</a> , et al. (25 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2401.15250v1-abstract-short" style="display: inline;"> Pump-probe experiments with sub-femtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of sub-femtosecond pulse pairs from a two-colour X-ray free-electron laser (XFEL). By measuring the delay between the two pulses with an angular streaking diagnostic, we characterise the group velocity of the XFEL and demonstrate… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2401.15250v1-abstract-full').style.display = 'inline'; document.getElementById('2401.15250v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2401.15250v1-abstract-full" style="display: none;"> Pump-probe experiments with sub-femtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of sub-femtosecond pulse pairs from a two-colour X-ray free-electron laser (XFEL). By measuring the delay between the two pulses with an angular streaking diagnostic, we characterise the group velocity of the XFEL and demonstrate control of the pulse delay down to 270 as. We demonstrate the application of this technique to a pump-probe measurement in core-excited para-aminophenol. These results demonstrate the ability to perform pump-probe experiments with sub-femtosecond resolution and atomic site specificity. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2401.15250v1-abstract-full').style.display = 'none'; document.getElementById('2401.15250v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 26 January, 2024; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> January 2024. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">55 pages, main manuscript (5 figures) + supplementary materials (25 figures), 30 figures total. Submitted to Nature Photonics</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2303.13940">arXiv:2303.13940</a> <span> [<a href="https://arxiv.org/pdf/2303.13940">pdf</a>, <a href="https://arxiv.org/format/2303.13940">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1088/1367-2630/acee19">10.1088/1367-2630/acee19 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Femtosecond pulse parameter estimation from photoelectron momenta using machine learning </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Szo%C5%82dra%2C+T">Tomasz Szo艂dra</a>, <a href="/search/physics?searchtype=author&query=Ciappina%2C+M+F">Marcelo F. Ciappina</a>, <a href="/search/physics?searchtype=author&query=Werby%2C+N">Nicholas Werby</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Lewenstein%2C+M">Maciej Lewenstein</a>, <a href="/search/physics?searchtype=author&query=Zakrzewski%2C+J">Jakub Zakrzewski</a>, <a href="/search/physics?searchtype=author&query=Maxwell%2C+A+S">Andrew S. Maxwell</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2303.13940v2-abstract-short" style="display: inline;"> Deep learning models have provided huge interpretation power for image-like data. Specifically, convolutional neural networks (CNNs) have demonstrated incredible acuity for tasks such as feature extraction or parameter estimation. Here we test CNNs on strong-field ionization photoelectron spectra, training on theoretical data sets to `invert' experimental data. Pulse characterization is used as a… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2303.13940v2-abstract-full').style.display = 'inline'; document.getElementById('2303.13940v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2303.13940v2-abstract-full" style="display: none;"> Deep learning models have provided huge interpretation power for image-like data. Specifically, convolutional neural networks (CNNs) have demonstrated incredible acuity for tasks such as feature extraction or parameter estimation. Here we test CNNs on strong-field ionization photoelectron spectra, training on theoretical data sets to `invert' experimental data. Pulse characterization is used as a `testing ground', specifically we retrieve the laser intensity, where `traditional' measurements typically lead to 20% uncertainty. We report on crucial data augmentation techniques required to successfully train on theoretical data and return consistent results from experiments, including accounting for detector saturation. The same procedure can be repeated to apply CNNs in a range of scenarios for strong-field ionization. Using a predictive uncertainty estimation, reliable laser intensity uncertainties of a few percent can be extracted, which are consistently lower than those given by traditional techniques. Using interpretability methods can reveal parts of the distribution that are most sensitive to laser intensity, which can be directly associated with holographic interferences. The CNNs employed provide an accurate and convenient ways to extract parameters, and represent a novel interpretational tool for strong-field ionization spectra. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2303.13940v2-abstract-full').style.display = 'none'; document.getElementById('2303.13940v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 18 October, 2023; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 24 March, 2023; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> March 2023. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">13 pages, 5 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> New J. Phys. 25, 083039 (2023) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2303.03586">arXiv:2303.03586</a> <span> [<a href="https://arxiv.org/pdf/2303.03586">pdf</a>, <a href="https://arxiv.org/format/2303.03586">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> </div> <p class="title is-5 mathjax"> Femtosecond electronic and hydrogen structural dynamics in ammonia imaged with ultrafast electron diffraction </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Champenois%2C+E+G">Elio G. Champenois</a>, <a href="/search/physics?searchtype=author&query=List%2C+N+H">Nanna H. List</a>, <a href="/search/physics?searchtype=author&query=Ware%2C+M">Matthew Ware</a>, <a href="/search/physics?searchtype=author&query=Britton%2C+M">Mathew Britton</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+X">Xinxin Cheng</a>, <a href="/search/physics?searchtype=author&query=Centurion%2C+M">Martin Centurion</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">Ruaridh Forbes</a>, <a href="/search/physics?searchtype=author&query=Gabalski%2C+I">Ian Gabalski</a>, <a href="/search/physics?searchtype=author&query=Hegazy%2C+K">Kareem Hegazy</a>, <a href="/search/physics?searchtype=author&query=Hoffmann%2C+M+C">Matthias C. Hoffmann</a>, <a href="/search/physics?searchtype=author&query=Howard%2C+A+J">Andrew J. Howard</a>, <a href="/search/physics?searchtype=author&query=Ji%2C+F">Fuhao Ji</a>, <a href="/search/physics?searchtype=author&query=Lin%2C+M">Ming-Fu Lin</a>, <a href="/search/physics?searchtype=author&query=Nunes%2C+J+P">J. Pedro Nunes</a>, <a href="/search/physics?searchtype=author&query=Shen%2C+X">Xiaozhe Shen</a>, <a href="/search/physics?searchtype=author&query=Yang%2C+J">Jie Yang</a>, <a href="/search/physics?searchtype=author&query=Wang%2C+X">Xijie Wang</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T+J">Todd J. Martinez</a>, <a href="/search/physics?searchtype=author&query=Wolf%2C+T+J+A">Thomas J. A. Wolf</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2303.03586v1-abstract-short" style="display: inline;"> Directly imaging structural dynamics involving hydrogen atoms by ultrafast diffraction methods is complicated by their low scattering cross-sections. Here we demonstrate that megaelectronvolt ultrafast electron diffraction is sufficiently sensitive to follow hydrogen dynamics in isolated molecules. In a study of the photodissociation of gas phase ammonia, we simultaneously observe signatures of th… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2303.03586v1-abstract-full').style.display = 'inline'; document.getElementById('2303.03586v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2303.03586v1-abstract-full" style="display: none;"> Directly imaging structural dynamics involving hydrogen atoms by ultrafast diffraction methods is complicated by their low scattering cross-sections. Here we demonstrate that megaelectronvolt ultrafast electron diffraction is sufficiently sensitive to follow hydrogen dynamics in isolated molecules. In a study of the photodissociation of gas phase ammonia, we simultaneously observe signatures of the nuclear and corresponding electronic structure changes resulting from the dissociation dynamics in the time-dependent diffraction. Both assignments are confirmed by ab initio simulations of the photochemical dynamics and the resulting diffraction observable. While the temporal resolution of the experiment is insufficient to resolve the dissociation in time, our results represent an important step towards the observation of proton dynamics in real space and time. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2303.03586v1-abstract-full').style.display = 'none'; document.getElementById('2303.03586v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 6 March, 2023; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> March 2023. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2210.13645">arXiv:2210.13645</a> <span> [<a href="https://arxiv.org/pdf/2210.13645">pdf</a>, <a href="https://arxiv.org/format/2210.13645">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> </div> <p class="title is-5 mathjax"> Filming Enhanced Ionization in an Ultrafast Triatomic Slingshot </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Howard%2C+A+J">A. J. Howard</a>, <a href="/search/physics?searchtype=author&query=Britton%2C+M">M. Britton</a>, <a href="/search/physics?searchtype=author&query=Streeter%2C+Z+L">Z. L. Streeter</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+C">C. Cheng</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">R. Forbes</a>, <a href="/search/physics?searchtype=author&query=Reynolds%2C+J+L">J. L. Reynolds</a>, <a href="/search/physics?searchtype=author&query=Allum%2C+F">F. Allum</a>, <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">G. A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Gabalski%2C+I">I. Gabalski</a>, <a href="/search/physics?searchtype=author&query=Lucchese%2C+R+R">R. R. Lucchese</a>, <a href="/search/physics?searchtype=author&query=McCurdy%2C+C+W">C. W. McCurdy</a>, <a href="/search/physics?searchtype=author&query=Weinacht%2C+T">T. Weinacht</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2210.13645v1-abstract-short" style="display: inline;"> Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e. filmed)… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2210.13645v1-abstract-full').style.display = 'inline'; document.getElementById('2210.13645v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2210.13645v1-abstract-full" style="display: none;"> Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e. filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid "slingshot" motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2210.13645v1-abstract-full').style.display = 'none'; document.getElementById('2210.13645v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 24 October, 2022; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> October 2022. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2210.09480">arXiv:2210.09480</a> <span> [<a href="https://arxiv.org/pdf/2210.09480">pdf</a>, <a href="https://arxiv.org/format/2210.09480">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Data Analysis, Statistics and Probability">physics.data-an</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1088/1367-2630/acc201">10.1088/1367-2630/acc201 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Photon Energy-Resolved Velocity Map Imaging from Spectral Domain Ghost Imaging </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Wang%2C+J">Jun Wang</a>, <a href="/search/physics?searchtype=author&query=Driver%2C+T+C">Taran C. Driver</a>, <a href="/search/physics?searchtype=author&query=Allum%2C+F">Felix Allum</a>, <a href="/search/physics?searchtype=author&query=Papadopoulou%2C+C+C">Christina C. Papadopoulou</a>, <a href="/search/physics?searchtype=author&query=Passow%2C+C">Christopher Passow</a>, <a href="/search/physics?searchtype=author&query=Brenner%2C+G">G眉nter Brenner</a>, <a href="/search/physics?searchtype=author&query=Li%2C+S">Siqi Li</a>, <a href="/search/physics?searchtype=author&query=D%C3%BCsterer%2C+S">Stefan D眉sterer</a>, <a href="/search/physics?searchtype=author&query=Noor%2C+A+T">Atia Tul Noor</a>, <a href="/search/physics?searchtype=author&query=Kumar%2C+S">Sonu Kumar</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Erk%2C+B">Benjamin Erk</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">Ruaridh Forbes</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2210.09480v2-abstract-short" style="display: inline;"> We present an approach that combines photon spectrum correlation analysis with the reconstruction of three-dimensional momentum distribution from velocity map images in an efficient, single-step procedure. We demonstrate its efficacy with the results from the photoionization of the $2p$-shell of argon using the FLASH free-electron laser~(FEL). Distinct spectral features due to the spin-orbit split… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2210.09480v2-abstract-full').style.display = 'inline'; document.getElementById('2210.09480v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2210.09480v2-abstract-full" style="display: none;"> We present an approach that combines photon spectrum correlation analysis with the reconstruction of three-dimensional momentum distribution from velocity map images in an efficient, single-step procedure. We demonstrate its efficacy with the results from the photoionization of the $2p$-shell of argon using the FLASH free-electron laser~(FEL). Distinct spectral features due to the spin-orbit splitting of Ar$^+(2p^{-1})$ are resolved, despite the large average bandwidth of the ionizing pulses from the FEL. This demonstrates a clear advantage over the conventional analysis method, and it will be broadly beneficial for velocity map imaging experiments with FEL sources. The retrieved linewidth of the binding energy spectrum approaches the resolution limitation prescribed by the spectrometers used to collect the data. Our approach presents a path to extend spectral-domain ghost imaging to the case where the photoproduct observable is high-dimensional. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2210.09480v2-abstract-full').style.display = 'none'; document.getElementById('2210.09480v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 20 March, 2023; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 17 October, 2022; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> October 2022. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">14 pages</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> New J. Phys. 25 033017 (2023) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2205.07166">arXiv:2205.07166</a> <span> [<a href="https://arxiv.org/pdf/2205.07166">pdf</a>, <a href="https://arxiv.org/format/2205.07166">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> </div> <p class="title is-5 mathjax"> Time Correlation Filtering Reveals Two-Path Electron Quantum Interference in Strong-Field Ionization </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Werby%2C+N">Nicholas Werby</a>, <a href="/search/physics?searchtype=author&query=Maxwell%2C+A+S">Andrew S. Maxwell</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">Ruaridh Forbes</a>, <a href="/search/physics?searchtype=author&query=Faria%2C+C+F+d+M">Carla Figueira de Morisson Faria</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2205.07166v1-abstract-short" style="display: inline;"> Attosecond dynamics in strong-field tunnel ionization are encoded in intricate holographic patterns in the photoelectron momentum distributions (PMDs). These patterns show the interference between two or more superposed quantum electron trajectories, which are defined by their ionization times and subsequent evolution in the laser field. We determine the ionization time separation between interfer… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2205.07166v1-abstract-full').style.display = 'inline'; document.getElementById('2205.07166v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2205.07166v1-abstract-full" style="display: none;"> Attosecond dynamics in strong-field tunnel ionization are encoded in intricate holographic patterns in the photoelectron momentum distributions (PMDs). These patterns show the interference between two or more superposed quantum electron trajectories, which are defined by their ionization times and subsequent evolution in the laser field. We determine the ionization time separation between interfering pairs of electron orbits by performing a differential Fourier analysis on the measured momentum spectrum. We identify electron holograms formed by trajectory pairs whose ionization times are separated by less than a single quarter cycle, between a quarter cycle and half cycle, between a half cycle and three fourths of a cycle, and a full cycle apart. We compare our experimental results to the predictions of the Coulomb quantum orbit strong-field approximation (CQSFA), with significant success. We also time-filter the CQSFA trajectory calculations to demonstrate the validity of the technique on spectra with known time correlations. As a general analysis technique, the filter can be applied to all energy- and angularly-resolved datasets to recover time correlations between interfering electron pathways, providing an important tool to analyze any strong-field ionization spectra. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2205.07166v1-abstract-full').style.display = 'none'; document.getElementById('2205.07166v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 14 May, 2022; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> May 2022. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">11 pages, 7 figures, submitted to Physical Review X</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2107.03697">arXiv:2107.03697</a> <span> [<a href="https://arxiv.org/pdf/2107.03697">pdf</a>, <a href="https://arxiv.org/format/2107.03697">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="High Energy Physics - Experiment">hep-ex</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Instrumentation and Detectors">physics.ins-det</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1088/1367-2630/ac4283">10.1088/1367-2630/ac4283 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Single Particle Detection System for Strong-Field QED Experiments </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Salgado%2C+F+C">F. C. Salgado</a>, <a href="/search/physics?searchtype=author&query=Cavanagh%2C+N">N. Cavanagh</a>, <a href="/search/physics?searchtype=author&query=Tamburini%2C+M">M. Tamburini</a>, <a href="/search/physics?searchtype=author&query=Storey%2C+D+W">D. W. Storey</a>, <a href="/search/physics?searchtype=author&query=Beyer%2C+R">R. Beyer</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Chen%2C+Z">Z. Chen</a>, <a href="/search/physics?searchtype=author&query=Di+Piazza%2C+A">A. Di Piazza</a>, <a href="/search/physics?searchtype=author&query=Gerstmayr%2C+E">E. Gerstmayr</a>, <a href="/search/physics?searchtype=author&query=Harsh"> Harsh</a>, <a href="/search/physics?searchtype=author&query=Isele%2C+E">E. Isele</a>, <a href="/search/physics?searchtype=author&query=Junghans%2C+A+R">A. R. Junghans</a>, <a href="/search/physics?searchtype=author&query=Keitel%2C+C+H">C. H. Keitel</a>, <a href="/search/physics?searchtype=author&query=Kuschel%2C+S">S. Kuschel</a>, <a href="/search/physics?searchtype=author&query=Nielsen%2C+C+F">C. F. Nielsen</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">D. A. Reis</a>, <a href="/search/physics?searchtype=author&query=Roedel%2C+C">C. Roedel</a>, <a href="/search/physics?searchtype=author&query=Sarri%2C+G">G. Sarri</a>, <a href="/search/physics?searchtype=author&query=Seidel%2C+A">A. Seidel</a>, <a href="/search/physics?searchtype=author&query=Schneider%2C+C">C. Schneider</a>, <a href="/search/physics?searchtype=author&query=Uggerh%C3%B8j%2C+U+I">U. I. Uggerh酶j</a>, <a href="/search/physics?searchtype=author&query=Wulff%2C+J">J. Wulff</a>, <a href="/search/physics?searchtype=author&query=Yakimenko%2C+V">V. Yakimenko</a>, <a href="/search/physics?searchtype=author&query=Zepter%2C+C">C. Zepter</a>, <a href="/search/physics?searchtype=author&query=Meuren%2C+S">S. Meuren</a> , et al. (1 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2107.03697v2-abstract-short" style="display: inline;"> Measuring signatures of strong-field quantum electrodynamics (SF-QED) processes in an intense laser field is an experimental challenge: it requires detectors to be highly sensitive to single electrons and positrons in the presence of the typically very strong x-ray and $纬$-photon background levels. In this paper, we describe a particle detector capable of diagnosing single leptons from SF-QED inte… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2107.03697v2-abstract-full').style.display = 'inline'; document.getElementById('2107.03697v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2107.03697v2-abstract-full" style="display: none;"> Measuring signatures of strong-field quantum electrodynamics (SF-QED) processes in an intense laser field is an experimental challenge: it requires detectors to be highly sensitive to single electrons and positrons in the presence of the typically very strong x-ray and $纬$-photon background levels. In this paper, we describe a particle detector capable of diagnosing single leptons from SF-QED interactions and discuss the background level simulations for the upcoming Experiment-320 at FACET-II (SLAC National Accelerator Laboratory). The single particle detection system described here combines pixelated scintillation LYSO screens and a Cherenkov calorimeter. We detail the performance of the system using simulations and a calibration of the Cherenkov detector at the ELBE accelerator. Single 3 GeV leptons are expected to produce approximately 537 detectable photons in a single calorimeter channel. This signal is compared to Monte-Carlo simulations of the experiment. A signal-to-noise ratio of 18 in a single Cherenkov calorimeter detector is expected and a spectral resolution of 2% is achieved using the pixelated LYSO screens. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2107.03697v2-abstract-full').style.display = 'none'; document.getElementById('2107.03697v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 9 December, 2021; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 8 July, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> July 2021. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> New J. Phys. 24, 015002 (2021) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2105.11607">arXiv:2105.11607</a> <span> [<a href="https://arxiv.org/pdf/2105.11607">pdf</a>, <a href="https://arxiv.org/ps/2105.11607">ps</a>, <a href="https://arxiv.org/format/2105.11607">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Plasma Physics">physics.plasm-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="High Energy Physics - Phenomenology">hep-ph</span> </div> </div> <p class="title is-5 mathjax"> MP3 White Paper 2021 -- Research Opportunities Enabled by Co-locating Multi-Petawatt Lasers with Dense Ultra-Relativistic Electron Beams </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Meuren%2C+S">Sebastian Meuren</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">David A. Reis</a>, <a href="/search/physics?searchtype=author&query=Blandford%2C+R">Roger Blandford</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Phil H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Fisch%2C+N+J">Nathaniel J. Fisch</a>, <a href="/search/physics?searchtype=author&query=Fiuza%2C+F">Frederico Fiuza</a>, <a href="/search/physics?searchtype=author&query=Gerstmayr%2C+E">Elias Gerstmayr</a>, <a href="/search/physics?searchtype=author&query=Glenzer%2C+S">Siegfried Glenzer</a>, <a href="/search/physics?searchtype=author&query=Hogan%2C+M+J">Mark J. Hogan</a>, <a href="/search/physics?searchtype=author&query=Pellegrini%2C+C">Claudio Pellegrini</a>, <a href="/search/physics?searchtype=author&query=Peskin%2C+M+E">Michael E. Peskin</a>, <a href="/search/physics?searchtype=author&query=Qu%2C+K">Kenan Qu</a>, <a href="/search/physics?searchtype=author&query=White%2C+G">Glen White</a>, <a href="/search/physics?searchtype=author&query=Yakimenko%2C+V">Vitaly Yakimenko</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2105.11607v1-abstract-short" style="display: inline;"> Novel emergent phenomena are expected to occur under conditions exceeding the QED critical electric field, where the vacuum becomes unstable to electron-positron pair production. The required intensity to reach this regime, $\sim10^{29}\,\mathrm{Wcm^{-2}}$, cannot be achieved even with the most intense lasers now being planned/constructed without a sizeable Lorentz boost provided by interactions w… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2105.11607v1-abstract-full').style.display = 'inline'; document.getElementById('2105.11607v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2105.11607v1-abstract-full" style="display: none;"> Novel emergent phenomena are expected to occur under conditions exceeding the QED critical electric field, where the vacuum becomes unstable to electron-positron pair production. The required intensity to reach this regime, $\sim10^{29}\,\mathrm{Wcm^{-2}}$, cannot be achieved even with the most intense lasers now being planned/constructed without a sizeable Lorentz boost provided by interactions with ultrarelativistic particles. Seeded laser-laser collisions may access this strong-field QED regime at laser intensities as low as $\sim10^{24}\,\mathrm{Wcm^{-2}}$. Counterpropagating e-beam--laser interactions exceed the QED critical field at still lower intensities ($\sim10^{20}\,\mathrm{Wcm^{-2}}$ at $\sim10\,\mathrm{GeV}$). Novel emergent phenomena are predicted to occur in the "QED plasma regime", where strong-field quantum and collective plasma effects play off one another. Here the electron beam density becomes a decisive factor. Thus, the challenge is not just to exceed the QED critical field, but to do so with high quality, approaching solid-density electron beams. Even though laser wakefield accelerators (LWFA) represent a very promising research field, conventional accelerators still provide orders of magnitude higher charge densities at energies $\gtrsim10\,\mathrm{GeV}$. Co-location of extremely dense and highly energetic electron beams with a multi-petawatt laser system would therefore enable seminal research opportunities in high-field physics and laboratory astrophysics. This white paper elucidates the potential scientific impact of multi-beam capabilities that combine a multi-PW optical laser, high-energy/density electron beam, and high-intensity x rays and outlines how to achieve such capabilities by co-locating a 3-10 PW laser with a state-of-the-art linear accelerator. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2105.11607v1-abstract-full').style.display = 'none'; document.getElementById('2105.11607v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 24 May, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> May 2021. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">3 pages</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2105.08854">arXiv:2105.08854</a> <span> [<a href="https://arxiv.org/pdf/2105.08854">pdf</a>, <a href="https://arxiv.org/format/2105.08854">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1126/science.abj2096">10.1126/science.abj2096 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Attosecond Coherent Electron Motion in Auger-Meitner Decay </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Li%2C+S">Siqi Li</a>, <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a>, <a href="/search/physics?searchtype=author&query=Rosenberger%2C+P">Philipp Rosenberger</a>, <a href="/search/physics?searchtype=author&query=Champenois%2C+E+G">Elio G. Champenois</a>, <a href="/search/physics?searchtype=author&query=Duris%2C+J">Joseph Duris</a>, <a href="/search/physics?searchtype=author&query=Al-Haddad%2C+A">Andre Al-Haddad</a>, <a href="/search/physics?searchtype=author&query=Averbukh%2C+V">Vitali Averbukh</a>, <a href="/search/physics?searchtype=author&query=Barnard%2C+J+C+T">Jonathan C. T. Barnard</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">Nora Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">Christoph Bostedt</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Coffee%2C+R">Ryan Coffee</a>, <a href="/search/physics?searchtype=author&query=DiMauro%2C+L+F">Louis F. DiMauro</a>, <a href="/search/physics?searchtype=author&query=Fang%2C+L">Li Fang</a>, <a href="/search/physics?searchtype=author&query=Garratt%2C+D">Douglas Garratt</a>, <a href="/search/physics?searchtype=author&query=Gatton%2C+A">Averell Gatton</a>, <a href="/search/physics?searchtype=author&query=Guo%2C+Z">Zhaoheng Guo</a>, <a href="/search/physics?searchtype=author&query=Hartmann%2C+G">Gregor Hartmann</a>, <a href="/search/physics?searchtype=author&query=Haxton%2C+D">Daniel Haxton</a>, <a href="/search/physics?searchtype=author&query=Helml%2C+W">Wolfram Helml</a>, <a href="/search/physics?searchtype=author&query=Huang%2C+Z">Zhirong Huang</a>, <a href="/search/physics?searchtype=author&query=LaForge%2C+A+C">Aaron C. LaForge</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a>, <a href="/search/physics?searchtype=author&query=Knurr%2C+J">Jonas Knurr</a>, <a href="/search/physics?searchtype=author&query=Lin%2C+M">Ming-Fu Lin</a> , et al. (16 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2105.08854v1-abstract-short" style="display: inline;"> In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond soft x-ray pulses produced by an x-ray free-electron laser to induce a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized i… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2105.08854v1-abstract-full').style.display = 'inline'; document.getElementById('2105.08854v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2105.08854v1-abstract-full" style="display: none;"> In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond soft x-ray pulses produced by an x-ray free-electron laser to induce a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse we create a clock to time-resolve the electron dynamics, and demonstrate control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2105.08854v1-abstract-full').style.display = 'none'; document.getElementById('2105.08854v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 18 May, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> May 2021. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2105.06507">arXiv:2105.06507</a> <span> [<a href="https://arxiv.org/pdf/2105.06507">pdf</a>, <a href="https://arxiv.org/format/2105.06507">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevX.11.031048">10.1103/PhysRevX.11.031048 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Correlation Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Barillot%2C+T">T. Barillot</a>, <a href="/search/physics?searchtype=author&query=Alexander%2C+O">O. Alexander</a>, <a href="/search/physics?searchtype=author&query=Cooper%2C+B">B. Cooper</a>, <a href="/search/physics?searchtype=author&query=Driver%2C+T">T. Driver</a>, <a href="/search/physics?searchtype=author&query=Garratt%2C+D">D. Garratt</a>, <a href="/search/physics?searchtype=author&query=Li%2C+S">S. Li</a>, <a href="/search/physics?searchtype=author&query=Haddad%2C+A+A">A. Al Haddad</a>, <a href="/search/physics?searchtype=author&query=Sanchez-Gonzalez%2C+A">A. Sanchez-Gonzalez</a>, <a href="/search/physics?searchtype=author&query=Ag%C3%A5ker%2C+M">M. Ag氓ker</a>, <a href="/search/physics?searchtype=author&query=Arrell%2C+C">C. Arrell</a>, <a href="/search/physics?searchtype=author&query=Bearpark%2C+M">M. Bearpark</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">N. Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">C. Bostedt</a>, <a href="/search/physics?searchtype=author&query=Bozek%2C+J">J. Bozek</a>, <a href="/search/physics?searchtype=author&query=Brahms%2C+C">C. Brahms</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Clark%2C+A">A. Clark</a>, <a href="/search/physics?searchtype=author&query=Doumy%2C+G">G. Doumy</a>, <a href="/search/physics?searchtype=author&query=Feifel%2C+R">R. Feifel</a>, <a href="/search/physics?searchtype=author&query=Frasinski%2C+L+J">L. J. Frasinski</a>, <a href="/search/physics?searchtype=author&query=Jarosch%2C+S">S. Jarosch</a>, <a href="/search/physics?searchtype=author&query=Johnson%2C+A+S">A. S. Johnson</a>, <a href="/search/physics?searchtype=author&query=Kjellsson%2C+L">L. Kjellsson</a>, <a href="/search/physics?searchtype=author&query=Koloren%C4%8D%2C+P">P. Koloren膷</a>, <a href="/search/physics?searchtype=author&query=Kumagai%2C+Y">Y. Kumagai</a> , et al. (24 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2105.06507v1-abstract-short" style="display: inline;"> The possibility of suddenly ionized molecules undergoing extremely fast electron hole dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecu… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2105.06507v1-abstract-full').style.display = 'inline'; document.getElementById('2105.06507v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2105.06507v1-abstract-full" style="display: none;"> The possibility of suddenly ionized molecules undergoing extremely fast electron hole dynamics prior to significant structural change was first recognized more than 20 years ago and termed charge migration. The accurate probing of ultrafast electron hole dynamics requires measurements that have both sufficient temporal resolution and can detect the localization of a specific hole within the molecule. We report an investigation of the dynamics of inner valence hole states in isopropanol where we use an x-ray pump/x-ray probe experiment, with site and state-specific probing of a transient hole state localized near the oxygen atom in the molecule, together with an ab initio theoretical treatment. We record the signature of transient hole dynamics and make the first observation of dynamics driven by frustrated Auger-Meitner transitions. We verify that the hole lifetime is consistent with our theoretical prediction. This state-specific measurement paves the way to widespread application for observations of transient hole dynamics localized in space and time in molecules and thus to charge transfer phenomena that are fundamental in chemical and material physics. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2105.06507v1-abstract-full').style.display = 'none'; document.getElementById('2105.06507v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 13 May, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> May 2021. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. X 11, 031048 (2021) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2104.05869">arXiv:2104.05869</a> <span> [<a href="https://arxiv.org/pdf/2104.05869">pdf</a>, <a href="https://arxiv.org/format/2104.05869">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevA.104.023108">10.1103/PhysRevA.104.023108 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Strong Field Ionization of Water II: Electronic and Nuclear Dynamics En Route to Double Ionization </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Cheng%2C+C">Chuan Cheng</a>, <a href="/search/physics?searchtype=author&query=Streeter%2C+Z+L">Zachary L. Streeter</a>, <a href="/search/physics?searchtype=author&query=Howard%2C+A+J">Andrew J. Howard</a>, <a href="/search/physics?searchtype=author&query=Spanner%2C+M">Michael Spanner</a>, <a href="/search/physics?searchtype=author&query=Lucchese%2C+R+R">Robert R. Lucchese</a>, <a href="/search/physics?searchtype=author&query=McCurdy%2C+C+W">C. William McCurdy</a>, <a href="/search/physics?searchtype=author&query=Weinacht%2C+T">Thomas Weinacht</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">Ruaridh Forbes</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2104.05869v2-abstract-short" style="display: inline;"> We investigate the role of nuclear motion and strong-field-induced electronic couplings during the double ionization of deuterated water using momentum-resolved coincidence spectroscopy. By examining the three-body dicationic dissociation channel, D$^{+}$/D$^{+}$/O, for both few- and multi-cycle laser pulses, strong evidence for intra-pulse dynamics is observed. The extracted angle- and energy-res… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2104.05869v2-abstract-full').style.display = 'inline'; document.getElementById('2104.05869v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2104.05869v2-abstract-full" style="display: none;"> We investigate the role of nuclear motion and strong-field-induced electronic couplings during the double ionization of deuterated water using momentum-resolved coincidence spectroscopy. By examining the three-body dicationic dissociation channel, D$^{+}$/D$^{+}$/O, for both few- and multi-cycle laser pulses, strong evidence for intra-pulse dynamics is observed. The extracted angle- and energy-resolved double ionization yields are compared to classical trajectory simulations of the dissociation dynamics occurring from different electronic states of the dication. In contrast with measurements of single photon double ionization, pronounced departure from the expectations for vertical ionization is observed, even for pulses as short as 10~fs in duration. We outline numerous mechanisms by which the strong laser field can modify the nuclear wavefunction en-route to final states of the dication where molecular fragmentation occurs. Specifically, we consider the possibility of a coordinate-dependence to the strong-field ionization rate, intermediate nuclear motion in monocation states prior to double ionization, and near-resonant laser-induced dipole couplings in the ion. These results highlight the fact that, for small and light molecules such as D$_2$O, a vertical-transition treatment of the ionization dynamics is not sufficient to reproduce the features seen experimentally in the strong field coincidence double-ionization data. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2104.05869v2-abstract-full').style.display = 'none'; document.getElementById('2104.05869v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 10 May, 2021; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 12 April, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> April 2021. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">14 pages, 13 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. A 104, 023108 (2021) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2102.12000">arXiv:2102.12000</a> <span> [<a href="https://arxiv.org/pdf/2102.12000">pdf</a>, <a href="https://arxiv.org/format/2102.12000">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevA.104.013109">10.1103/PhysRevA.104.013109 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Dissecting Sub-Cycle Interference in Photoelectron Holography </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Werby%2C+N">Nicholas Werby</a>, <a href="/search/physics?searchtype=author&query=Maxwell%2C+A+S">Andrew S. Maxwell</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">Ruaridh Forbes</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Faria%2C+C+F+d+M">Carla Figueira de Morisson Faria</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2102.12000v1-abstract-short" style="display: inline;"> Multipath holographic interference in strong-field quantum tunnel ionization is key to revealing sub-Angstrom attosecond dynamics for molecular movies. This critical sub-cycle motion is often obscured by longer time-scale effects such as ring-shaped patterns that appear in above-threshold ionization (ATI). In the present work, we overcome this problem by combining two novel techniques in theory an… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2102.12000v1-abstract-full').style.display = 'inline'; document.getElementById('2102.12000v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2102.12000v1-abstract-full" style="display: none;"> Multipath holographic interference in strong-field quantum tunnel ionization is key to revealing sub-Angstrom attosecond dynamics for molecular movies. This critical sub-cycle motion is often obscured by longer time-scale effects such as ring-shaped patterns that appear in above-threshold ionization (ATI). In the present work, we overcome this problem by combining two novel techniques in theory and experimental analysis: unit-cell averaging and time-filtering data and simulations. Together these suppress ATI rings and enable an unprecedented highly-detailed quantitative match between strong-field ionization experiments in argon and the Coulomb-quantum orbit strong-field approximation (CQSFA) theory. Velocity map images reveal fine modulations on the holographic spider-like interference fringes that form near the polarization axis. CQSFA theory traces this to the interference of three types of electron pathways. The level of agreement between experiment and theory allows sensitive determination of quantum phase differences and symmetries, providing an important tool for quantitative dynamical imaging in quantum systems. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2102.12000v1-abstract-full').style.display = 'none'; document.getElementById('2102.12000v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 23 February, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> February 2021. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">13 Pages, 8 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. A 104, 013109 (2021) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2101.12301">arXiv:2101.12301</a> <span> [<a href="https://arxiv.org/pdf/2101.12301">pdf</a>, <a href="https://arxiv.org/ps/2101.12301">ps</a>, <a href="https://arxiv.org/format/2101.12301">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevA.103.043120">10.1103/PhysRevA.103.043120 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Strong Field Ionization of Water: Nuclear Dynamics Revealed by Varying the Pulse Duration </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Howard%2C+A+J">A. J. Howard</a>, <a href="/search/physics?searchtype=author&query=Cheng%2C+C">C. Cheng</a>, <a href="/search/physics?searchtype=author&query=Forbes%2C+R">R. Forbes</a>, <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">G. A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Mills%2C+W+H">W. H. Mills</a>, <a href="/search/physics?searchtype=author&query=Makhija%2C+V">V. Makhija</a>, <a href="/search/physics?searchtype=author&query=Spanner%2C+M">M. Spanner</a>, <a href="/search/physics?searchtype=author&query=Weinacht%2C+T">T. Weinacht</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2101.12301v1-abstract-short" style="display: inline;"> Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2101.12301v1-abstract-full').style.display = 'inline'; document.getElementById('2101.12301v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2101.12301v1-abstract-full" style="display: none;"> Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (both H$_2$O and D$_2$O) in 10-fs and 40-fs 800-nm laser pulses. We find that 10-fs pulses turn off before substantial internuclear motion occurs, whereas rapid internuclear motion can take place during the double ionization process for 40-fs pulses. The short-pulse measurements are consistent with a simple tunnel ionization picture, whose predictions help interpret the motion observed in the long-pulse measurements. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2101.12301v1-abstract-full').style.display = 'none'; document.getElementById('2101.12301v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 28 January, 2021; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> January 2021. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">9 pages, 5 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. A 103, 043120 (2021) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2011.06761">arXiv:2011.06761</a> <span> [<a href="https://arxiv.org/pdf/2011.06761">pdf</a>, <a href="https://arxiv.org/format/2011.06761">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1039/D0FD00126K">10.1039/D0FD00126K <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Resolving Multiphoton Processes with High-Order Anisotropy Ultrafast X-ray Scattering </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Natan%2C+A">Adi Natan</a>, <a href="/search/physics?searchtype=author&query=Schori%2C+A">Aviad Schori</a>, <a href="/search/physics?searchtype=author&query=Owolabi%2C+G">Grace Owolabi</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">James M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2011.06761v3-abstract-short" style="display: inline;"> We present first results on ultrafast X-ray scattering of strongly driven molecular Iodine and analysis of high-order anisotropic components of the scattering signal, up to four-photon absorption. We discuss the technical details of retrieving high fidelity high-order anisotropy components, and outline a method to analyze the scattering signal using Legendre decomposition. We use simulated anisotr… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2011.06761v3-abstract-full').style.display = 'inline'; document.getElementById('2011.06761v3-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2011.06761v3-abstract-full" style="display: none;"> We present first results on ultrafast X-ray scattering of strongly driven molecular Iodine and analysis of high-order anisotropic components of the scattering signal, up to four-photon absorption. We discuss the technical details of retrieving high fidelity high-order anisotropy components, and outline a method to analyze the scattering signal using Legendre decomposition. We use simulated anisotropic scattering signals and Fourier analysis to map how anisotropic dissociation motions can be extracted from the various Legendre orders. We observe multitude dissociation and vibration motions simultaneously arising from various multiphoton transitions. We use the anisotropy information of the scattering signal to disentangle the different processes and assign their dissociation velocities on the Angstrom and femtosecond scales de-novo. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2011.06761v3-abstract-full').style.display = 'none'; document.getElementById('2011.06761v3-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 17 December, 2020; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 12 November, 2020; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> November 2020. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">20 pages, 6 figures</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2009.14355">arXiv:2009.14355</a> <span> [<a href="https://arxiv.org/pdf/2009.14355">pdf</a>, <a href="https://arxiv.org/format/2009.14355">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1039/D0FD00112K">10.1039/D0FD00112K <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Transient Resonant Auger-Meitner Spectra of Photoexcited Thymine </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Wolf%2C+T+J+A">Thomas J. A. Wolf</a>, <a href="/search/physics?searchtype=author&query=Paul%2C+A+C">Alexander C. Paul</a>, <a href="/search/physics?searchtype=author&query=Folkestad%2C+S+D">Sarai D. Folkestad</a>, <a href="/search/physics?searchtype=author&query=Myhre%2C+R+H">Rolf H. Myhre</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">Nora Berrah</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Phil H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Coriani%2C+S">Sonia Coriani</a>, <a href="/search/physics?searchtype=author&query=Coslovich%2C+G">Giacomo Coslovich</a>, <a href="/search/physics?searchtype=author&query=Feifel%2C+R">Raimund Feifel</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T+J">Todd J. Martinez</a>, <a href="/search/physics?searchtype=author&query=Moeller%2C+S+P">Stefan P. Moeller</a>, <a href="/search/physics?searchtype=author&query=Mucke%2C+M">Melanie Mucke</a>, <a href="/search/physics?searchtype=author&query=Obaid%2C+R">Razib Obaid</a>, <a href="/search/physics?searchtype=author&query=Plekan%2C+O">Oksana Plekan</a>, <a href="/search/physics?searchtype=author&query=Squibb%2C+R+J">Richard J. Squibb</a>, <a href="/search/physics?searchtype=author&query=Koch%2C+H">Henrik Koch</a>, <a href="/search/physics?searchtype=author&query=G%C3%BChr%2C+M">Markus G眉hr</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2009.14355v1-abstract-short" style="display: inline;"> We present the first investigation of excited state dynamics by resonant Auger-Meitner spectroscopy (also known as resonant Auger spectroscopy) using the nucleobase thymine as an example. Thymine is photoexcited in the UV and probed with X-ray photon energies at and below the oxygen K-edge. After initial photoexcitation to a 蟺蟺* excited state, thymine is known to undergo internal conversion to an… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2009.14355v1-abstract-full').style.display = 'inline'; document.getElementById('2009.14355v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2009.14355v1-abstract-full" style="display: none;"> We present the first investigation of excited state dynamics by resonant Auger-Meitner spectroscopy (also known as resonant Auger spectroscopy) using the nucleobase thymine as an example. Thymine is photoexcited in the UV and probed with X-ray photon energies at and below the oxygen K-edge. After initial photoexcitation to a 蟺蟺* excited state, thymine is known to undergo internal conversion to an n蟺* excited state with a strong resonance at the oxygen K-edge, red-shifted from the ground state 蟺* resonances of thymine (see our previous study Wolf et al., Nat. Commun., 2017, 8, 29). We resolve and compare the Auger-Meitner electron spectra associated both with the excited state and ground state resonances, and distinguish participator and spectator decay contributions. Furthermore, we observe simultaneously with the decay of the n蟺* state signatures the appearance of additional resonant Auger-Meitner contributions at photon energies between the n蟺* state and the ground state resonances. We assign these contributions to population transfer from the n蟺* state to a 蟺蟺* triplet state via intersystem crossing on the picosecond timescale based on simulations of the X-ray absorption spectra in the vibrationally hot triplet state. Moreover, we identify signatures from the initially excited 蟺蟺* singlet state which we have not observed in our previous study. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2009.14355v1-abstract-full').style.display = 'none'; document.getElementById('2009.14355v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 29 September, 2020; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> September 2020. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2006.14724">arXiv:2006.14724</a> <span> [<a href="https://arxiv.org/pdf/2006.14724">pdf</a>, <a href="https://arxiv.org/format/2006.14724">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> </div> <p class="title is-5 mathjax"> Nonlinear resonant X-ray Raman scattering </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Haber%2C+J">Johann Haber</a>, <a href="/search/physics?searchtype=author&query=Kaldun%2C+A">Andreas Kaldun</a>, <a href="/search/physics?searchtype=author&query=Teitelbaum%2C+S+W">Samuel W. Teitelbaum</a>, <a href="/search/physics?searchtype=author&query=Baron%2C+A+Q+R">Alfred Q. R. Baron</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Fuchs%2C+M">Matthias Fuchs</a>, <a href="/search/physics?searchtype=author&query=Hastings%2C+J+B">Jerome B. Hastings</a>, <a href="/search/physics?searchtype=author&query=Inoue%2C+I">Ichiro Inoue</a>, <a href="/search/physics?searchtype=author&query=Inubushi%2C+Y">Yuichi Inubushi</a>, <a href="/search/physics?searchtype=author&query=Krebs%2C+D">Dietrich Krebs</a>, <a href="/search/physics?searchtype=author&query=Osaka%2C+T">Taito Osaka</a>, <a href="/search/physics?searchtype=author&query=Santra%2C+R">Robin Santra</a>, <a href="/search/physics?searchtype=author&query=Shwartz%2C+S">Sharon Shwartz</a>, <a href="/search/physics?searchtype=author&query=Tamasaku%2C+K">Kenji Tamasaku</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">David A. Reis</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2006.14724v1-abstract-short" style="display: inline;"> We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises m… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2006.14724v1-abstract-full').style.display = 'inline'; document.getElementById('2006.14724v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2006.14724v1-abstract-full" style="display: none;"> We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2006.14724v1-abstract-full').style.display = 'none'; document.getElementById('2006.14724v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 25 June, 2020; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> June 2020. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">6 pages, 4 figures</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2003.02096">arXiv:2003.02096</a> <span> [<a href="https://arxiv.org/pdf/2003.02096">pdf</a>, <a href="https://arxiv.org/format/2003.02096">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1063/5.0007058">10.1063/5.0007058 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Strictly Non-Adiabatic Quantum Control of the Acetylene Dication Using an Infrared Field </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Liekhus-Schmaltz%2C+C">Chelsea Liekhus-Schmaltz</a>, <a href="/search/physics?searchtype=author&query=Zhu%2C+X">Xiaolei Zhu</a>, <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">Gregory A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T">Todd Martinez</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2003.02096v1-abstract-short" style="display: inline;"> We demonstrate the existence of a strictly non-adiabatic control pathway in deprotonation of the acetylene dication. This pathway is identified experimentally by measuring a kinetic energy shift in an ion coincidence experiment. We use a TDSE simulation to identify which properties most strongly affect our control. We find that resonant control around conical intersections is limited by the speed… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2003.02096v1-abstract-full').style.display = 'inline'; document.getElementById('2003.02096v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2003.02096v1-abstract-full" style="display: none;"> We demonstrate the existence of a strictly non-adiabatic control pathway in deprotonation of the acetylene dication. This pathway is identified experimentally by measuring a kinetic energy shift in an ion coincidence experiment. We use a TDSE simulation to identify which properties most strongly affect our control. We find that resonant control around conical intersections is limited by the speed of non-adiabatic dynamics. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2003.02096v1-abstract-full').style.display = 'none'; document.getElementById('2003.02096v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 20 January, 2020; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> March 2020. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">7 pages, 3 figures</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/2002.10051">arXiv:2002.10051</a> <span> [<a href="https://arxiv.org/pdf/2002.10051">pdf</a>, <a href="https://arxiv.org/format/2002.10051">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Plasma Physics">physics.plasm-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="High Energy Physics - Phenomenology">hep-ph</span> </div> </div> <p class="title is-5 mathjax"> On Seminal HEDP Research Opportunities Enabled by Colocating Multi-Petawatt Laser with High-Density Electron Beams </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Meuren%2C+S">Sebastian Meuren</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Phil H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Fisch%2C+N+J">Nathaniel J. Fisch</a>, <a href="/search/physics?searchtype=author&query=Fi%C3%BAza%2C+F">Frederico Fi煤za</a>, <a href="/search/physics?searchtype=author&query=Glenzer%2C+S">Siegfried Glenzer</a>, <a href="/search/physics?searchtype=author&query=Hogan%2C+M+J">Mark J. Hogan</a>, <a href="/search/physics?searchtype=author&query=Qu%2C+K">Kenan Qu</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">David A. Reis</a>, <a href="/search/physics?searchtype=author&query=White%2C+G">Glen White</a>, <a href="/search/physics?searchtype=author&query=Yakimenko%2C+V">Vitaly Yakimenko</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="2002.10051v1-abstract-short" style="display: inline;"> The scientific community is currently witnessing an expensive and worldwide race to achieve the highest possible light intensity. Within the next decade this effort is expected to reach nearly $10^{24}\,\mathrm{W}/\mathrm{cm^2}$ in the lab frame by focusing of 100 PW, near-infrared lasers. A major driving force behind this effort is the possibility to study strong-field vacuum breakdown and an acc… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2002.10051v1-abstract-full').style.display = 'inline'; document.getElementById('2002.10051v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="2002.10051v1-abstract-full" style="display: none;"> The scientific community is currently witnessing an expensive and worldwide race to achieve the highest possible light intensity. Within the next decade this effort is expected to reach nearly $10^{24}\,\mathrm{W}/\mathrm{cm^2}$ in the lab frame by focusing of 100 PW, near-infrared lasers. A major driving force behind this effort is the possibility to study strong-field vacuum breakdown and an accompanying electron-positron pair plasma via a quantum electrodynamic (QED) cascade [Edwin Cartlidge, "The light fantastic", Science 359, 382 (2018)]. Whereas Europe is focusing on all-optical 10 PW-class laser facilities (e.g., Apollon and ELI), China is already planning on co-locating a 100 PW laser system with a 25 keV superconducting XFEL and thus implicitly also a high-quality electron beam [Station of Extreme Light (SEL) at the Shanghai Superintense-Ultrafast Lasers Facility (SULF)]. This white paper elucidates the seminal scientific opportunities facilitated by colliding dense, multi-GeV electron beams with multi-PW optical laser pulses. Such a multi-beam facility would enable the experimental exploration of extreme HEDP environments by generating electron-positron pair plasmas with unprecedented densities and temperatures, where the interplay between strong-field quantum and collective plasma effects becomes decisive. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('2002.10051v1-abstract-full').style.display = 'none'; document.getElementById('2002.10051v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 23 February, 2020; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> February 2020. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">11 pages, 1 figure, 1 table</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1911.01323">arXiv:1911.01323</a> <span> [<a href="https://arxiv.org/pdf/1911.01323">pdf</a>, <a href="https://arxiv.org/format/1911.01323">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevX.10.011065">10.1103/PhysRevX.10.011065 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Characterizing multiphoton excitation using time-resolved X-ray scattering </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Ware%2C+M+R">Matthew R. Ware</a>, <a href="/search/physics?searchtype=author&query=Natan%2C+A">Adi Natan</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">James M. Glownia</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1911.01323v1-abstract-short" style="display: inline;"> Molecular iodine was photoexcited by a strong 800 nm laser, driving several channels of multiphoton excitation. The motion following photoexcitation was probed using time-resolved X-ray scattering, which produces a scattering map $S(Q,蟿)$. Temporal Fourier transform methods were employed to obtain a frequency-resolved X-ray scattering signal $\tilde{S}(Q,蠅)$. Taken together, $S(Q,蟿)$ and… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1911.01323v1-abstract-full').style.display = 'inline'; document.getElementById('1911.01323v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1911.01323v1-abstract-full" style="display: none;"> Molecular iodine was photoexcited by a strong 800 nm laser, driving several channels of multiphoton excitation. The motion following photoexcitation was probed using time-resolved X-ray scattering, which produces a scattering map $S(Q,蟿)$. Temporal Fourier transform methods were employed to obtain a frequency-resolved X-ray scattering signal $\tilde{S}(Q,蠅)$. Taken together, $S(Q,蟿)$ and $\tilde{S}(Q,蠅)$ separate different modes of motion, so that mode-specific nuclear oscillatory positions, oscillation amplitudes, directions of motions, and times may be measured accurately. Molecular dissociations likewise have a distinct signature, which may be used to identify both velocities and dissociation time shifts, and also can reveal laser-induced couplings among the molecular potentials. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1911.01323v1-abstract-full').style.display = 'none'; document.getElementById('1911.01323v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 4 November, 2019; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> November 2019. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. X 10, 011065 (2020) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1909.07441">arXiv:1909.07441</a> <span> [<a href="https://arxiv.org/pdf/1909.07441">pdf</a>, <a href="https://arxiv.org/format/1909.07441">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1039/C9CP03951A">10.1039/C9CP03951A <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Attosecond Transient Absorption Spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Driver%2C+T">Taran Driver</a>, <a href="/search/physics?searchtype=author&query=Li%2C+S">Siqi Li</a>, <a href="/search/physics?searchtype=author&query=Champenois%2C+E+G">Elio G. Champenois</a>, <a href="/search/physics?searchtype=author&query=Duris%2C+J">Joseph Duris</a>, <a href="/search/physics?searchtype=author&query=Ratner%2C+D">Daniel Ratner</a>, <a href="/search/physics?searchtype=author&query=Lane%2C+T">TJ Lane</a>, <a href="/search/physics?searchtype=author&query=Rosenberger%2C+P">Philipp Rosenberger</a>, <a href="/search/physics?searchtype=author&query=Al-Haddad%2C+A">Andre Al-Haddad</a>, <a href="/search/physics?searchtype=author&query=Averbukh%2C+V">Vitali Averbukh</a>, <a href="/search/physics?searchtype=author&query=Barnard%2C+T">Toby Barnard</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">Nora Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">Christoph Bostedt</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Coffee%2C+R">Ryan Coffee</a>, <a href="/search/physics?searchtype=author&query=DiMauro%2C+L+F">Louis F. DiMauro</a>, <a href="/search/physics?searchtype=author&query=Fang%2C+L">Li Fang</a>, <a href="/search/physics?searchtype=author&query=Garratt%2C+D">Douglas Garratt</a>, <a href="/search/physics?searchtype=author&query=Gatton%2C+A">Averell Gatton</a>, <a href="/search/physics?searchtype=author&query=Guo%2C+Z">Zhaoheng Guo</a>, <a href="/search/physics?searchtype=author&query=Hartmann%2C+G">Gregor Hartmann</a>, <a href="/search/physics?searchtype=author&query=Haxton%2C+D">Daniel Haxton</a>, <a href="/search/physics?searchtype=author&query=Helml%2C+W">Wolfram Helml</a>, <a href="/search/physics?searchtype=author&query=Huang%2C+Z">Zhirong Huang</a>, <a href="/search/physics?searchtype=author&query=LaForge%2C+A">Aaron LaForge</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a> , et al. (16 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1909.07441v1-abstract-short" style="display: inline;"> The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the result… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1909.07441v1-abstract-full').style.display = 'inline'; document.getElementById('1909.07441v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1909.07441v1-abstract-full" style="display: none;"> The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1909.07441v1-abstract-full').style.display = 'none'; document.getElementById('1909.07441v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 16 September, 2019; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> September 2019. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">13 pages, 3 figures</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1906.10728">arXiv:1906.10728</a> <span> [<a href="https://arxiv.org/pdf/1906.10728">pdf</a>, <a href="https://arxiv.org/format/1906.10728">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevA.102.023118">10.1103/PhysRevA.102.023118 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Electron Correlation Effects in Attosecond Photoionization of CO$_{2}$ </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a>, <a href="/search/physics?searchtype=author&query=Wang%2C+A+L">Anna L. Wang</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Haxton%2C+D+J">Daniel J. Haxton</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1906.10728v1-abstract-short" style="display: inline;"> A technique for measuring photoionization time delays with attosecond precision is combined with calculations of photoionization matrix elements to demonstrate how multi-electron dynamics affect photoionization time delays in carbon dioxide. Electron correlation is observed to affect the time delays through two mechanisms: autoionization of molecular Rydberg states and accelerated escape from a co… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1906.10728v1-abstract-full').style.display = 'inline'; document.getElementById('1906.10728v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1906.10728v1-abstract-full" style="display: none;"> A technique for measuring photoionization time delays with attosecond precision is combined with calculations of photoionization matrix elements to demonstrate how multi-electron dynamics affect photoionization time delays in carbon dioxide. Electron correlation is observed to affect the time delays through two mechanisms: autoionization of molecular Rydberg states and accelerated escape from a continuum shape resonance. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1906.10728v1-abstract-full').style.display = 'none'; document.getElementById('1906.10728v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 25 June, 2019; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> June 2019. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. A 102, 023118 (2020) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1905.02821">arXiv:1905.02821</a> <span> [<a href="https://arxiv.org/pdf/1905.02821">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> </div> <p class="title is-5 mathjax"> Overcoming the absorption limit in high-harmonic generation from crystals </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Liu%2C+H">Hanzhe Liu</a>, <a href="/search/physics?searchtype=author&query=Vampa%2C+G">Giulio Vampa</a>, <a href="/search/physics?searchtype=author&query=Zhang%2C+J+L">Jingyuan Linda Zhang</a>, <a href="/search/physics?searchtype=author&query=Shi%2C+Y">Yu Shi</a>, <a href="/search/physics?searchtype=author&query=Buddhiraju%2C+S">Siddharth Buddhiraju</a>, <a href="/search/physics?searchtype=author&query=Fan%2C+S">Shanhui Fan</a>, <a href="/search/physics?searchtype=author&query=Vuckovic%2C+J">Jelena Vuckovic</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">David A. Reis</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1905.02821v1-abstract-short" style="display: inline;"> Since the new millennium coherent extreme ultra-violet and soft x-ray radiation has revolutionized the understanding of dynamical physical, chemical and biological systems at the electron's natural timescale. Unfortunately, coherent laser-based upconversion of infrared photons to vacuum-ultraviolet and soft x-ray high-order harmonics in gaseous, liquid and solid targets is notoriously inefficient.… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1905.02821v1-abstract-full').style.display = 'inline'; document.getElementById('1905.02821v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1905.02821v1-abstract-full" style="display: none;"> Since the new millennium coherent extreme ultra-violet and soft x-ray radiation has revolutionized the understanding of dynamical physical, chemical and biological systems at the electron's natural timescale. Unfortunately, coherent laser-based upconversion of infrared photons to vacuum-ultraviolet and soft x-ray high-order harmonics in gaseous, liquid and solid targets is notoriously inefficient. In dense nonlinear media, the limiting factor is strong re-absorption of the generated high-energy photons. Here we overcome this limitation by allowing high-order harmonics generated from a periodic array of thin one-dimensional crystalline silicon ridge waveguides to propagate in the vacuum gaps between the ridges, thereby avoiding the high absorption loss of the bulk nonlinear material and resulting in a ~ 100-fold increase in propagation length. As the grating period is varied, each high-harmonic shows a different and marked modulation, indicating the onset of coherent addition which is otherwise suppressed in absorption-limited emission. By beating the absorption limit, our results pave the way for bright coherent short-wavelength sources and their implementation in nano-photonic devices. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1905.02821v1-abstract-full').style.display = 'none'; document.getElementById('1905.02821v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 7 May, 2019; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> May 2019. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1903.02824">arXiv:1903.02824</a> <span> [<a href="https://arxiv.org/pdf/1903.02824">pdf</a>, <a href="https://arxiv.org/format/1903.02824">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> </div> <p class="title is-5 mathjax"> Multiple Fourier Component Analysis of X-ray Second Harmonic Generation in Diamond </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Chakraborti%2C+P">P. Chakraborti</a>, <a href="/search/physics?searchtype=author&query=Senfftleben%2C+B">B. Senfftleben</a>, <a href="/search/physics?searchtype=author&query=Kettle%2C+B">B. Kettle</a>, <a href="/search/physics?searchtype=author&query=Teitelbaum%2C+S+W">S. W. Teitelbaum</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Ghimire%2C+S">S. Ghimire</a>, <a href="/search/physics?searchtype=author&query=Hastings%2C+J+B">J. B. Hastings</a>, <a href="/search/physics?searchtype=author&query=Liu%2C+H">H. Liu</a>, <a href="/search/physics?searchtype=author&query=Nelson%2C+S">S. Nelson</a>, <a href="/search/physics?searchtype=author&query=Sato%2C+T">T. Sato</a>, <a href="/search/physics?searchtype=author&query=Shwartz%2C+S">S. Shwartz</a>, <a href="/search/physics?searchtype=author&query=Sun%2C+Y">Y. Sun</a>, <a href="/search/physics?searchtype=author&query=Weninger%2C+C">C. Weninger</a>, <a href="/search/physics?searchtype=author&query=Zhu%2C+D">D. Zhu</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">D. A. Reis</a>, <a href="/search/physics?searchtype=author&query=Fuchs%2C+M">M. Fuchs</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1903.02824v1-abstract-short" style="display: inline;"> The unprecedented brilliance of X-ray free-electron lasers (XFELs) [1, 2] has enabled first studies of nonlinear interactions in the hard X-ray range. In particular, X-ray-optical mixing [3], X-ray second harmonic generation (XSHG) [4] and nonlinear Compton scattering (NLCS) [5] have been recently observed for the first time using XFELs. The former two experiments as well as X-ray parametric downc… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1903.02824v1-abstract-full').style.display = 'inline'; document.getElementById('1903.02824v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1903.02824v1-abstract-full" style="display: none;"> The unprecedented brilliance of X-ray free-electron lasers (XFELs) [1, 2] has enabled first studies of nonlinear interactions in the hard X-ray range. In particular, X-ray-optical mixing [3], X-ray second harmonic generation (XSHG) [4] and nonlinear Compton scattering (NLCS) [5] have been recently observed for the first time using XFELs. The former two experiments as well as X-ray parametric downconversion (XPDC)[6, 7] are well explained by nonlinearities in the impulse approximation[8], where electrons in a solid target are assumed to be quasi free for X-ray interactions far from atomic resonances. However, the energy of the photons generated in NLCS at intensities reaching up to 4 x 1020 W/cm2 exhibit an anomalous red-shift that is in violation with the free-electron model. Here we investigate the underlying physics of X-ray nonlinear interactions at intensities on order of 1016 W/cm2. Specifically, we perform a systematic study of XSHG in diamond. While one phase-matching geometry has been measured in Shwartz et al.[4], we extend these studies to multiple Fourier components and with significantly higher statistics, which allows us to determine the second order nonlinear structure factor. We measure the efficiency, angular dependence, and contributions from different source terms of the process. We find good agreement of our measurements with the quasi-free electron model. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1903.02824v1-abstract-full').style.display = 'none'; document.getElementById('1903.02824v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 7 March, 2019; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> March 2019. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1710.04244">arXiv:1710.04244</a> <span> [<a href="https://arxiv.org/pdf/1710.04244">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1038/s41567-018-0233-6">10.1038/s41567-018-0233-6 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Enhanced High-Harmonic Generation from an All-Dielectric Metasurface </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Liu%2C+H">Hanzhe Liu</a>, <a href="/search/physics?searchtype=author&query=Guo%2C+C">Cheng Guo</a>, <a href="/search/physics?searchtype=author&query=Vampa%2C+G">Giulio Vampa</a>, <a href="/search/physics?searchtype=author&query=Zhang%2C+J+L">Jingyuan Linda Zhang</a>, <a href="/search/physics?searchtype=author&query=Sarmiento%2C+T">Tomas Sarmiento</a>, <a href="/search/physics?searchtype=author&query=Xiao%2C+M">Meng Xiao</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Vu%C4%8Dkovi%C4%87%2C+J">Jelena Vu膷kovi膰</a>, <a href="/search/physics?searchtype=author&query=Fan%2C+S">Shanhui Fan</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">David A. Reis</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1710.04244v1-abstract-short" style="display: inline;"> The recent observation of high-harmonic generation from solids creates a new possibility for engineering fundamental strong-field processes by patterning the solid target with subwavelength nanostructures. All-dielectric metasurfaces exhibit high damage thresholds and strong enhancement of the driving field, making them attractive platforms to control high-harmonics and other high-field processes… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1710.04244v1-abstract-full').style.display = 'inline'; document.getElementById('1710.04244v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1710.04244v1-abstract-full" style="display: none;"> The recent observation of high-harmonic generation from solids creates a new possibility for engineering fundamental strong-field processes by patterning the solid target with subwavelength nanostructures. All-dielectric metasurfaces exhibit high damage thresholds and strong enhancement of the driving field, making them attractive platforms to control high-harmonics and other high-field processes at nanoscales. Here we report enhanced non-perturbative high-harmonic emission from a Si metasurface that possesses a sharp Fano resonance resulting from a classical analogue of electromagnetically induced transparency. Harmonic emission is enhanced by more than two orders of magnitude compared to unpatterned samples. The enhanced high harmonics are highly anisotropic with excitation polarization and are selective to excitation wavelength due to its resonant feature. By combining nanofabrication technology and ultrafast strong-field physics, our work paves the way for designing new compact ultrafast photonic devices that operate under high intensities and short wavelengths. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1710.04244v1-abstract-full').style.display = 'none'; document.getElementById('1710.04244v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 11 October, 2017; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> October 2017. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">14 pages, 4 figures</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1708.07214">arXiv:1708.07214</a> <span> [<a href="https://arxiv.org/pdf/1708.07214">pdf</a>, <a href="https://arxiv.org/ps/1708.07214">ps</a>, <a href="https://arxiv.org/format/1708.07214">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic and Molecular Clusters">physics.atm-clus</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1063/1.4997253">10.1063/1.4997253 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Geometric Dependence of Strong Field Enhanced Ionization in D$_{2}$O </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">Gregory A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Kaldun%2C+A">Andreas Kaldun</a>, <a href="/search/physics?searchtype=author&query=Liekhus-Schmaltz%2C+C">Chelsea Liekhus-Schmaltz</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1708.07214v1-abstract-short" style="display: inline;"> We have studied strong-field enhanced dissociative ionization of D$_{2}$O in 40 fs, 800 nm laser pulses with focused intensities of $< 1 - 3 \times 10^{15}W/cm^2$ by resolving the charged fragment momenta with respect to the laser polarization. We observe dication dissociation into OD$^{+}$/D$^{+}$ dominates when the polarization is out of the plane of the molecule, whereas trication dissociation… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1708.07214v1-abstract-full').style.display = 'inline'; document.getElementById('1708.07214v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1708.07214v1-abstract-full" style="display: none;"> We have studied strong-field enhanced dissociative ionization of D$_{2}$O in 40 fs, 800 nm laser pulses with focused intensities of $< 1 - 3 \times 10^{15}W/cm^2$ by resolving the charged fragment momenta with respect to the laser polarization. We observe dication dissociation into OD$^{+}$/D$^{+}$ dominates when the polarization is out of the plane of the molecule, whereas trication dissociation into O$^{+}$/D$^{+}$/D$^{+}$ is strongly dominant when the polarization is aligned along the D-D axis. Dication dissociation into O/D$^{+}$/D$^{+}$, and O$^{+}$/D$_2$$^{+}$ is not seen, nor is there any significant fragmentation into multiple ions when the laser is polarized along the C$_{2v}$ symmetry axis of the molecule. Even below the saturation intensity for OD$^{+}$/D$^{+}$, the O$^{+}$/D$^{+}$/D$^{+}$ channel has higher yield. By analyzing how the laser field is oriented within the molecular frame for both channels, we show that enhanced ionization is driving the triply charged three body breakup, but is not active for the doubly charged two body breakup. We conclude that laser-induced distortion of the molecular potential suppresses multiple ionization along the C$_{2v}$ axis, but enhances ionization along the D-D direction. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1708.07214v1-abstract-full').style.display = 'none'; document.getElementById('1708.07214v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 23 August, 2017; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> August 2017. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1708.03847">arXiv:1708.03847</a> <span> [<a href="https://arxiv.org/pdf/1708.03847">pdf</a>, <a href="https://arxiv.org/format/1708.03847">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> </div> <p class="title is-5 mathjax"> Filming non-radiative population transfer: Time-resolved x-ray scattering near an avoided crossing </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Ware%2C+M+R">Matthew R. Ware</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">James M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Hartsock%2C+R">Robert Hartsock</a>, <a href="/search/physics?searchtype=author&query=Natan%2C+A">Adi Natan</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1708.03847v3-abstract-short" style="display: inline;"> We show that time-resolved x-ray scattering from molecules prepared in a superposition of electronic states moving through an avoided crossing has new features not found in diffraction from the corresponding classical mixed state. Photoabsorption in molecular iodine at 520 nm produces a superposition of two dipole-allowed nearly degenerate electronic states, which interact due to non-adiabatic cou… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1708.03847v3-abstract-full').style.display = 'inline'; document.getElementById('1708.03847v3-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1708.03847v3-abstract-full" style="display: none;"> We show that time-resolved x-ray scattering from molecules prepared in a superposition of electronic states moving through an avoided crossing has new features not found in diffraction from the corresponding classical mixed state. Photoabsorption in molecular iodine at 520 nm produces a superposition of two dipole-allowed nearly degenerate electronic states, which interact due to non-adiabatic coupling. We show experimental evidence that the mixing of the nuclear wavepackets from the two electronic states at the avoided crossing leads to ultrafast changes in the angular composition of the scattering pattern. This provides a novel means to study transitions in excited molecular systems. We reconstruct a movie of the nuclear probability density arising from this interference. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1708.03847v3-abstract-full').style.display = 'none'; document.getElementById('1708.03847v3-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 15 November, 2017; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 12 August, 2017; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> August 2017. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1610.03378">arXiv:1610.03378</a> <span> [<a href="https://arxiv.org/pdf/1610.03378">pdf</a>, <a href="https://arxiv.org/format/1610.03378">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Data Analysis, Statistics and Probability">physics.data-an</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Accelerator Physics">physics.acc-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Machine Learning">stat.ML</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1038/ncomms15461">10.1038/ncomms15461 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Machine learning applied to single-shot x-ray diagnostics in an XFEL </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Sanchez-Gonzalez%2C+A">A. Sanchez-Gonzalez</a>, <a href="/search/physics?searchtype=author&query=Micaelli%2C+P">P. Micaelli</a>, <a href="/search/physics?searchtype=author&query=Olivier%2C+C">C. Olivier</a>, <a href="/search/physics?searchtype=author&query=Barillot%2C+T+R">T. R. Barillot</a>, <a href="/search/physics?searchtype=author&query=Ilchen%2C+M">M. Ilchen</a>, <a href="/search/physics?searchtype=author&query=Lutman%2C+A+A">A. A. Lutman</a>, <a href="/search/physics?searchtype=author&query=Marinelli%2C+A">A. Marinelli</a>, <a href="/search/physics?searchtype=author&query=Maxwell%2C+T">T. Maxwell</a>, <a href="/search/physics?searchtype=author&query=Achner%2C+A">A. Achner</a>, <a href="/search/physics?searchtype=author&query=Ag%C3%A5ker%2C+M">M. Ag氓ker</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">N. Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">C. Bostedt</a>, <a href="/search/physics?searchtype=author&query=Buck%2C+J">J. Buck</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Montero%2C+S+C">S. Carron Montero</a>, <a href="/search/physics?searchtype=author&query=Cooper%2C+B">B. Cooper</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">J. P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Dong%2C+M">M. Dong</a>, <a href="/search/physics?searchtype=author&query=Feifel%2C+R">R. Feifel</a>, <a href="/search/physics?searchtype=author&query=Frasinski%2C+L+J">L. J. Frasinski</a>, <a href="/search/physics?searchtype=author&query=Fukuzawa%2C+H">H. Fukuzawa</a>, <a href="/search/physics?searchtype=author&query=Galler%2C+A">A. Galler</a>, <a href="/search/physics?searchtype=author&query=Hartmann%2C+G">G. Hartmann</a>, <a href="/search/physics?searchtype=author&query=Hartmann%2C+N">N. Hartmann</a>, <a href="/search/physics?searchtype=author&query=Helml%2C+W">W. Helml</a> , et al. (17 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1610.03378v1-abstract-short" style="display: inline;"> X-ray free-electron lasers (XFELs) are the only sources currently able to produce bright few-fs pulses with tunable photon energies from 100 eV to more than 10 keV. Due to the stochastic SASE operating principles and other technical issues the output pulses are subject to large fluctuations, making it necessary to characterize the x-ray pulses on every shot for data sorting purposes. We present a… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1610.03378v1-abstract-full').style.display = 'inline'; document.getElementById('1610.03378v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1610.03378v1-abstract-full" style="display: none;"> X-ray free-electron lasers (XFELs) are the only sources currently able to produce bright few-fs pulses with tunable photon energies from 100 eV to more than 10 keV. Due to the stochastic SASE operating principles and other technical issues the output pulses are subject to large fluctuations, making it necessary to characterize the x-ray pulses on every shot for data sorting purposes. We present a technique that applies machine learning tools to predict x-ray pulse properties using simple electron beam and x-ray parameters as input. Using this technique at the Linac Coherent Light Source (LCLS), we report mean errors below 0.3 eV for the prediction of the photon energy at 530 eV and below 1.6 fs for the prediction of the delay between two x-ray pulses. We also demonstrate spectral shape prediction with a mean agreement of 97%. This approach could potentially be used at the next generation of high-repetition-rate XFELs to provide accurate knowledge of complex x-ray pulses at the full repetition rate. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1610.03378v1-abstract-full').style.display = 'none'; document.getElementById('1610.03378v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 11 October, 2016; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> October 2016. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">12 pages, 8 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Nature Communications 8, 15461 (2017) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1610.01190">arXiv:1610.01190</a> <span> [<a href="https://arxiv.org/pdf/1610.01190">pdf</a>, <a href="https://arxiv.org/format/1610.01190">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> </div> <p class="title is-5 mathjax"> The attosecond regime of impulsive stimulated electronic Raman excitation </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Ware%2C+M+R">Matthew R. Ware</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Haxton%2C+D+J">Daniel J. Haxton</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1610.01190v1-abstract-short" style="display: inline;"> We have calculated the resonant and nonresonant contributions to attosecond impulsive stimulated electronic Raman scattering (SERS) in regions of autoionizing transitions. Comparison with Multiconfiguration Time-Dependent Hartree-Fock (MCTDHF) calculations find that attosecond SERS is dominated by continuum transitions and not autoionizing resonances. These results agree quantitatively with a rate… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1610.01190v1-abstract-full').style.display = 'inline'; document.getElementById('1610.01190v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1610.01190v1-abstract-full" style="display: none;"> We have calculated the resonant and nonresonant contributions to attosecond impulsive stimulated electronic Raman scattering (SERS) in regions of autoionizing transitions. Comparison with Multiconfiguration Time-Dependent Hartree-Fock (MCTDHF) calculations find that attosecond SERS is dominated by continuum transitions and not autoionizing resonances. These results agree quantitatively with a rate equation that includes second-order Raman and first-and second-order photoionization rates. Such rate models can be extended to larger molecular systems. Our results indicate that attosecond SERS transition probabilities may be understood in terms of two-photon generalized cross sections even in the high-intensity limit for extreme ultraviolet wavelengths. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1610.01190v1-abstract-full').style.display = 'none'; document.getElementById('1610.01190v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 4 October, 2016; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> October 2016. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1608.03039">arXiv:1608.03039</a> <span> [<a href="https://arxiv.org/pdf/1608.03039">pdf</a>, <a href="https://arxiv.org/ps/1608.03039">ps</a>, <a href="https://arxiv.org/format/1608.03039">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevLett.117.153003">10.1103/PhysRevLett.117.153003 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Self-referenced coherent diffraction x-ray movie of Angstrom- and femtosecond-scale atomic motion </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">J. M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Natan%2C+A">A. Natan</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">J. P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Hartsock%2C+R">R. Hartsock</a>, <a href="/search/physics?searchtype=author&query=Kozina%2C+M">M. Kozina</a>, <a href="/search/physics?searchtype=author&query=Minitti%2C+M+P">M. P. Minitti</a>, <a href="/search/physics?searchtype=author&query=Nelson%2C+S">S. Nelson</a>, <a href="/search/physics?searchtype=author&query=Robinson%2C+J">J. Robinson</a>, <a href="/search/physics?searchtype=author&query=Sato%2C+T">T. Sato</a>, <a href="/search/physics?searchtype=author&query=van+Driel%2C+T">T. van Driel</a>, <a href="/search/physics?searchtype=author&query=Welch%2C+G">G. Welch</a>, <a href="/search/physics?searchtype=author&query=Weninger%2C+C">C. Weninger</a>, <a href="/search/physics?searchtype=author&query=Zhi%2C+D">D. Zhi</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1608.03039v3-abstract-short" style="display: inline;"> Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with time and space resolution of $30~$fs and $0.3$ 脜. The high spatial fidelity is due to interference between the moving excitation and the static initial charge distribution. This x-ray interference has not been employed to image internal motion in molecul… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1608.03039v3-abstract-full').style.display = 'inline'; document.getElementById('1608.03039v3-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1608.03039v3-abstract-full" style="display: none;"> Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with time and space resolution of $30~$fs and $0.3$ 脜. The high spatial fidelity is due to interference between the moving excitation and the static initial charge distribution. This x-ray interference has not been employed to image internal motion in molecules before. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on 脜ngstrom and femtosecond scales. Coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1608.03039v3-abstract-full').style.display = 'none'; document.getElementById('1608.03039v3-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 31 August, 2016; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 10 August, 2016; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> August 2016. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">Accepted by Physical Review Letters</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. Lett. 117, 153003 (2016) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1607.02558">arXiv:1607.02558</a> <span> [<a href="https://arxiv.org/pdf/1607.02558">pdf</a>, <a href="https://arxiv.org/ps/1607.02558">ps</a>, <a href="https://arxiv.org/format/1607.02558">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic and Molecular Clusters">physics.atm-clus</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1063/1.4964392">10.1063/1.4964392 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Coherent control using kinetic energy and the geometric phase of a conical intersection </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Liekhus-Schmaltz%2C+C">Chelsea Liekhus-Schmaltz</a>, <a href="/search/physics?searchtype=author&query=McCracken%2C+G+A">Gregory A. McCracken</a>, <a href="/search/physics?searchtype=author&query=Kaldun%2C+A">Andreas Kaldun</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1607.02558v2-abstract-short" style="display: inline;"> Conical intersections (CI) between molecular potential energy surfaces with non-vanishing non-adiabatic couplings generally occur in any molecule consisting of at least three atoms. They play a fundamental role in describing the molecular dynamics beyond the Born-Oppenheimer approximation and have been used to understand a large variety of effects, from photofragmentation and isomerization to more… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1607.02558v2-abstract-full').style.display = 'inline'; document.getElementById('1607.02558v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1607.02558v2-abstract-full" style="display: none;"> Conical intersections (CI) between molecular potential energy surfaces with non-vanishing non-adiabatic couplings generally occur in any molecule consisting of at least three atoms. They play a fundamental role in describing the molecular dynamics beyond the Born-Oppenheimer approximation and have been used to understand a large variety of effects, from photofragmentation and isomerization to more exotic applications such as exciton fission in semiconductors. However, few studies have used the features of a CI as a tool for coherent control. Here we demonstrate two modes of control around a conical intersection. The first uses a continuous light field to control the population on the two intersecting electronic states in the vicinity of a CI. The second uses a pulsed light field to control wavepackets that are subjected to the geometric phase shift in transit around a CI. This second technique is likely to be useful for studying the role of nuclear dynamics in electronic coherence phenomena. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1607.02558v2-abstract-full').style.display = 'none'; document.getElementById('1607.02558v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 4 August, 2016; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 8 July, 2016; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> July 2016. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1606.02663">arXiv:1606.02663</a> <span> [<a href="https://arxiv.org/pdf/1606.02663">pdf</a>, <a href="https://arxiv.org/ps/1606.02663">ps</a>, <a href="https://arxiv.org/format/1606.02663">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic and Molecular Clusters">physics.atm-clus</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevA.95.061403">10.1103/PhysRevA.95.061403 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Imaging the Breakdown of Molecular-Frame Dynamics through Rotational Uncoupling </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Zipp%2C+L+J">Lucas J. Zipp</a>, <a href="/search/physics?searchtype=author&query=Natan%2C+A">Adi Natan</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1606.02663v2-abstract-short" style="display: inline;"> We demonstrate the breakdown of molecular-frame dynamics induced by the uncoupling of molecular rotation from electronic motion in molecular Rydberg states. We observe this non-Born-Oppenheimer regime in the time domain through photoelectron imaging of a coherent molecular Rydberg wave packet in $\textrm{N}_2$. The photoelectron angular distribution shows a radically different time evolution than… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1606.02663v2-abstract-full').style.display = 'inline'; document.getElementById('1606.02663v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1606.02663v2-abstract-full" style="display: none;"> We demonstrate the breakdown of molecular-frame dynamics induced by the uncoupling of molecular rotation from electronic motion in molecular Rydberg states. We observe this non-Born-Oppenheimer regime in the time domain through photoelectron imaging of a coherent molecular Rydberg wave packet in $\textrm{N}_2$. The photoelectron angular distribution shows a radically different time evolution than that of a typical molecular-frame-fixed electron orbital, revealing the uncoupled motion of the electron as it precesses around the $averaged$ anisotropic potential of the rotating ion-core. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1606.02663v2-abstract-full').style.display = 'none'; document.getElementById('1606.02663v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 4 July, 2017; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 8 June, 2016; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> June 2016. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">6 pages, 4 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. A 95, 061403 (2017) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1511.05626">arXiv:1511.05626</a> <span> [<a href="https://arxiv.org/pdf/1511.05626">pdf</a>, <a href="https://arxiv.org/ps/1511.05626">ps</a>, <a href="https://arxiv.org/format/1511.05626">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic and Molecular Clusters">physics.atm-clus</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevLett.116.143004">10.1103/PhysRevLett.116.143004 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Observation of Quantum Interferences via Light Induced Conical Intersections in Diatomic Molecules </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Natan%2C+A">Adi Natan</a>, <a href="/search/physics?searchtype=author&query=Ware%2C+M+R">Matthew R Ware</a>, <a href="/search/physics?searchtype=author&query=Prabhudesai%2C+V+S">Vaibhav S. Prabhudesai</a>, <a href="/search/physics?searchtype=author&query=Lev%2C+U">Uri Lev</a>, <a href="/search/physics?searchtype=author&query=Bruner%2C+B+D">Barry D. Bruner</a>, <a href="/search/physics?searchtype=author&query=Heber%2C+O">Oded Heber</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1511.05626v2-abstract-short" style="display: inline;"> We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H$_2^+$. The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed 2-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1511.05626v2-abstract-full').style.display = 'inline'; document.getElementById('1511.05626v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1511.05626v2-abstract-full" style="display: none;"> We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H$_2^+$. The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed 2-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a strong laser field. The interference magnitude and angular period depend strongly on the energy difference between the initial state and the LICI, consistent with coherent diffraction around a cone-shaped potential barrier whose width and thickness depend on the relative energy of the initial state and the cone apex. These findings are supported by numerical solutions of the time-dependent Schr枚dinger equation for similar experimental conditions. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1511.05626v2-abstract-full').style.display = 'none'; document.getElementById('1511.05626v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 26 January, 2016; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 17 November, 2015; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> November 2015. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">4 pages, 4 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. Lett. 116, 143004 (2016) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1504.06811">arXiv:1504.06811</a> <span> [<a href="https://arxiv.org/pdf/1504.06811">pdf</a>, <a href="https://arxiv.org/ps/1504.06811">ps</a>, <a href="https://arxiv.org/format/1504.06811">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevLett.115.203002">10.1103/PhysRevLett.115.203002 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Observation of Bloch oscillations in molecular rotation </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Flo%C3%9F%2C+J">Johannes Flo脽</a>, <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a>, <a href="/search/physics?searchtype=author&query=Averbukh%2C+I+S">Ilya Sh. Averbukh</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1504.06811v1-abstract-short" style="display: inline;"> The periodically kicked quantum rotor is known for non-classical effects such as quantum localisation in angular momentum space or quantum resonances in rotational excitation. These phenomena have been studied in diverse systems mimicking the kicked rotor, such as cold atoms in optical lattices, or coupled photonic structures. Recently, it was predicted that several solid state quantum localisatio… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1504.06811v1-abstract-full').style.display = 'inline'; document.getElementById('1504.06811v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1504.06811v1-abstract-full" style="display: none;"> The periodically kicked quantum rotor is known for non-classical effects such as quantum localisation in angular momentum space or quantum resonances in rotational excitation. These phenomena have been studied in diverse systems mimicking the kicked rotor, such as cold atoms in optical lattices, or coupled photonic structures. Recently, it was predicted that several solid state quantum localisation phenomena - Anderson localisation, Bloch oscillations, and Tamm-Shockley surface states - may manifest themselves in the rotational dynamics of laser-kicked molecules. Here, we report the first observation of rotational Bloch oscillations in a gas of nitrogen molecules kicked by a periodic train of femtosecond laser pulses. A controllable detuning from the quantum resonance creates an effective accelerating potential in angular momentum space, inducing Bloch-like oscillations of the rotational excitation. These oscillations are measured via the temporal modulation of the refractive index of the gas. Our results introduce room-temperature laser-kicked molecules as a new laboratory for studies of localisation phenomena in quantum transport. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1504.06811v1-abstract-full').style.display = 'none'; document.getElementById('1504.06811v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 26 April, 2015; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> April 2015. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">5 pages, 5 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Phys. Rev. Lett. 115, 203002 (2015) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1502.00704">arXiv:1502.00704</a> <span> [<a href="https://arxiv.org/pdf/1502.00704">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Instrumentation and Detectors">physics.ins-det</span> </div> </div> <p class="title is-5 mathjax"> Nonlinear X-ray Compton Scattering </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Fuchs%2C+M">Matthias Fuchs</a>, <a href="/search/physics?searchtype=author&query=Trigo%2C+M">Mariano Trigo</a>, <a href="/search/physics?searchtype=author&query=Chen%2C+J">Jian Chen</a>, <a href="/search/physics?searchtype=author&query=Ghimire%2C+S">Shambhu Ghimire</a>, <a href="/search/physics?searchtype=author&query=Shwartz%2C+S">Sharon Shwartz</a>, <a href="/search/physics?searchtype=author&query=Kozina%2C+M">Michael Kozina</a>, <a href="/search/physics?searchtype=author&query=Jiang%2C+M">Mason Jiang</a>, <a href="/search/physics?searchtype=author&query=Henighan%2C+T">Thomas Henighan</a>, <a href="/search/physics?searchtype=author&query=Bray%2C+C">Crystal Bray</a>, <a href="/search/physics?searchtype=author&query=Ndabashimiye%2C+G">Georges Ndabashimiye</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Feng%2C+Y">Yiping Feng</a>, <a href="/search/physics?searchtype=author&query=Herrmann%2C+S">Sven Herrmann</a>, <a href="/search/physics?searchtype=author&query=Carini%2C+G">Gabriella Carini</a>, <a href="/search/physics?searchtype=author&query=Pines%2C+J">Jack Pines</a>, <a href="/search/physics?searchtype=author&query=Hart%2C+P">Philip Hart</a>, <a href="/search/physics?searchtype=author&query=Kenney%2C+C">Christopher Kenney</a>, <a href="/search/physics?searchtype=author&query=Guillet%2C+S">Serge Guillet</a>, <a href="/search/physics?searchtype=author&query=Boutet%2C+S">Sebastien Boutet</a>, <a href="/search/physics?searchtype=author&query=Williams%2C+G">Garth Williams</a>, <a href="/search/physics?searchtype=author&query=Messerschmidt%2C+M">Marc Messerschmidt</a>, <a href="/search/physics?searchtype=author&query=Seibert%2C+M">Marvin Seibert</a>, <a href="/search/physics?searchtype=author&query=Moeller%2C+S">Stefan Moeller</a>, <a href="/search/physics?searchtype=author&query=Hastings%2C+J+B">Jerome B. Hastings</a>, <a href="/search/physics?searchtype=author&query=Reis%2C+D+A">David A. Reis</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1502.00704v2-abstract-short" style="display: inline;"> X-ray scattering is a weak linear probe of matter. It is primarily sensitive to the position of electrons and their momentum distribution. Elastic X-ray scattering forms the basis of atomic structural determination while inelastic Compton scattering is often used as a spectroscopic probe of both single-particle excitations and collective modes. X-ray free-electron lasers (XFELs) are unique tools f… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1502.00704v2-abstract-full').style.display = 'inline'; document.getElementById('1502.00704v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1502.00704v2-abstract-full" style="display: none;"> X-ray scattering is a weak linear probe of matter. It is primarily sensitive to the position of electrons and their momentum distribution. Elastic X-ray scattering forms the basis of atomic structural determination while inelastic Compton scattering is often used as a spectroscopic probe of both single-particle excitations and collective modes. X-ray free-electron lasers (XFELs) are unique tools for studying matter on its natural time and length scales due to their bright and coherent ultrashort pulses. However, in the focus of an XFEL the assumption of a weak linear probe breaks down, and nonlinear light-matter interactions can become ubiquitous. The field can be sufficiently high that even non-resonant multiphoton interactions at hard X-rays wavelengths become relevant. Here we report the observation of one of the most fundamental nonlinear X-ray-matter interactions, the simultaneous Compton scattering of two identical photons producing a single photon at nearly twice the photon energy. We measure scattered photons with an energy near 18 keV generated from solid beryllium irradiated by 8.8-9.75 keV XFEL pulses. The intensity in the X-ray focus reaches up to 4x20 W/cm2, which corresponds to a peak electric field two orders of magnitude higher than the atomic unit of field-strength and within four orders of magnitude of the quantum electrodynamic critical field. The observed signal scales quadratically in intensity and is emitted into a non-dipolar pattern, consistent with the simultaneous two-photon scattering from free electrons. However, the energy of the generated photons shows an anomalously large redshift only present at high intensities. This indicates that the instantaneous high-intensity scattering effectively interacts with a different electron momentum distribution than linear Compton scattering, with implications for the study of atomic-scale structure and dynamics of matter <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1502.00704v2-abstract-full').style.display = 'none'; document.getElementById('1502.00704v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 27 February, 2015; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 2 February, 2015; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> February 2015. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1501.04136">arXiv:1501.04136</a> <span> [<a href="https://arxiv.org/pdf/1501.04136">pdf</a>, <a href="https://arxiv.org/ps/1501.04136">ps</a>, <a href="https://arxiv.org/format/1501.04136">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Optics">physics.optics</span> </div> </div> <p class="title is-5 mathjax"> Dynamical Localization in Molecular Alignment of Kicked Quantum Rotors </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Kamalov%2C+A">Andrei Kamalov</a>, <a href="/search/physics?searchtype=author&query=Broege%2C+D+W">Douglas W. Broege</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1501.04136v2-abstract-short" style="display: inline;"> The periodically $未$-kicked quantum linear rotor is known to experience non-classical bounded energy growth due to quantum dynamical localization in angular momentum space. We study the effect of random deviations of the kick period in simulations and experiments. This breaks the energy and angular momentum localization and increases the rotational alignment, which is the analog of the onset of An… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1501.04136v2-abstract-full').style.display = 'inline'; document.getElementById('1501.04136v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1501.04136v2-abstract-full" style="display: none;"> The periodically $未$-kicked quantum linear rotor is known to experience non-classical bounded energy growth due to quantum dynamical localization in angular momentum space. We study the effect of random deviations of the kick period in simulations and experiments. This breaks the energy and angular momentum localization and increases the rotational alignment, which is the analog of the onset of Anderson localization in 1-D chains. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1501.04136v2-abstract-full').style.display = 'none'; document.getElementById('1501.04136v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 31 March, 2015; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 16 January, 2015; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> January 2015. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1308.3733">arXiv:1308.3733</a> <span> [<a href="https://arxiv.org/pdf/1308.3733">pdf</a>, <a href="https://arxiv.org/format/1308.3733">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> </div> <p class="title is-5 mathjax"> Multiple orbital contributions to molecular high-harmonic generation in an asymmetric top </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Spector%2C+L+S">Limor S. Spector</a>, <a href="/search/physics?searchtype=author&query=Miyabe%2C+S">Shungo Miyabe</a>, <a href="/search/physics?searchtype=author&query=Magana%2C+A">Alvaro Magana</a>, <a href="/search/physics?searchtype=author&query=Petretti%2C+S">Simon Petretti</a>, <a href="/search/physics?searchtype=author&query=Decleva%2C+P">Piero Decleva</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T">Todd Martinez</a>, <a href="/search/physics?searchtype=author&query=Saenz%2C+A">Alejandro Saenz</a>, <a href="/search/physics?searchtype=author&query=Guehr%2C+M">Markus Guehr</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1308.3733v1-abstract-short" style="display: inline;"> High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular geometries. Our measurements of the asymmetric top SO2 show large axis dependencies, which change with harmonic order. The analysis shows that these spectral fe… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1308.3733v1-abstract-full').style.display = 'inline'; document.getElementById('1308.3733v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1308.3733v1-abstract-full" style="display: none;"> High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular geometries. Our measurements of the asymmetric top SO2 show large axis dependencies, which change with harmonic order. The analysis shows that these spectral features must be due to field ionization and recombination from multiple orbitals during HHG. We expect that HHG can probe orbital dependencies using this approach for a broad class of asymmetric-top molecules. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1308.3733v1-abstract-full').style.display = 'none'; document.getElementById('1308.3733v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 16 August, 2013; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> August 2013. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">Main text and supplemental material</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1303.1429">arXiv:1303.1429</a> <span> [<a href="https://arxiv.org/pdf/1303.1429">pdf</a>, <a href="https://arxiv.org/ps/1303.1429">ps</a>, <a href="https://arxiv.org/format/1303.1429">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Accelerator Physics">physics.acc-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevLett.105.083005">10.1103/PhysRevLett.105.083005 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Double core hole production in N2: Beating the Auger clock </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Fang%2C+L">L. Fang</a>, <a href="/search/physics?searchtype=author&query=Hoener%2C+M">M. Hoener</a>, <a href="/search/physics?searchtype=author&query=Gessner%2C+O">O. Gessner</a>, <a href="/search/physics?searchtype=author&query=Tarantelli%2C+F">F. Tarantelli</a>, <a href="/search/physics?searchtype=author&query=Pratt%2C+S+T">S. T. Pratt</a>, <a href="/search/physics?searchtype=author&query=Kornilov%2C+O">O. Kornilov</a>, <a href="/search/physics?searchtype=author&query=Buth%2C+C">C. Buth</a>, <a href="/search/physics?searchtype=author&query=G%C3%BCehr%2C+M">M. G眉ehr</a>, <a href="/search/physics?searchtype=author&query=Kanter%2C+E+P">E. P. Kanter</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">C. Bostedt</a>, <a href="/search/physics?searchtype=author&query=Bozek%2C+J+D">J. D. Bozek</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Chen%2C+M">M. Chen</a>, <a href="/search/physics?searchtype=author&query=Coffee%2C+R">R. Coffee</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J">J. Cryan</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+M">M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Kukk%2C+E">E. Kukk</a>, <a href="/search/physics?searchtype=author&query=Leone%2C+S+R">S. R. Leone</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">N. Berrah</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1303.1429v1-abstract-short" style="display: inline;"> We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a timescale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron laser. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of doub… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1303.1429v1-abstract-full').style.display = 'inline'; document.getElementById('1303.1429v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1303.1429v1-abstract-full" style="display: none;"> We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a timescale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron laser. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of double core holes are expected, the first with two core holes on the same N atom, and the second with one core hole on each N atom. We report the first direct observations of the former type of core hole in a molecule, in good agreement with theory, and provide an experimental upper bound for the relative contribution of the latter type. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1303.1429v1-abstract-full').style.display = 'none'; document.getElementById('1303.1429v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 6 March, 2013; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> March 2013. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">5 pages, 3 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> PRL 105, 083005 (2010) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1301.6459">arXiv:1301.6459</a> <span> [<a href="https://arxiv.org/pdf/1301.6459">pdf</a>, <a href="https://arxiv.org/ps/1301.6459">ps</a>, <a href="https://arxiv.org/format/1301.6459">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Accelerator Physics">physics.acc-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevLett.109.263001">10.1103/PhysRevLett.109.263001 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Multiphoton Ionization as a clock to Reveal Molecular Dynamics with Intense Short X-ray Free Electron Laser Pulses </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Fang%2C+L">L. Fang</a>, <a href="/search/physics?searchtype=author&query=Osipov%2C+T">T. Osipov</a>, <a href="/search/physics?searchtype=author&query=Murphy%2C+B">B. Murphy</a>, <a href="/search/physics?searchtype=author&query=Tarantelli%2C+F">F. Tarantelli</a>, <a href="/search/physics?searchtype=author&query=Kukk%2C+E">E. Kukk</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">J. P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+M">M. Glownia</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Coffee%2C+R+N">R. N. Coffee</a>, <a href="/search/physics?searchtype=author&query=Chen%2C+M">M. Chen</a>, <a href="/search/physics?searchtype=author&query=Buth%2C+C">C. Buth</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">N. Berrah</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1301.6459v3-abstract-short" style="display: inline;"> We investigate molecular dynamics of multiple ionization in N2 through multiple core-level photoabsorption and subsequent Auger decay processes induced by intense, short X-ray free electron laser pulses. The timing dynamics of the photoabsorption and dissociation processes is mapped onto the kinetic energy of the fragments. Measurements of the latter allow us to map out the average internuclear se… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1301.6459v3-abstract-full').style.display = 'inline'; document.getElementById('1301.6459v3-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1301.6459v3-abstract-full" style="display: none;"> We investigate molecular dynamics of multiple ionization in N2 through multiple core-level photoabsorption and subsequent Auger decay processes induced by intense, short X-ray free electron laser pulses. The timing dynamics of the photoabsorption and dissociation processes is mapped onto the kinetic energy of the fragments. Measurements of the latter allow us to map out the average internuclear separation for every molecular photoionization sequence step and obtain the average time interval between the photoabsorption events. Using multiphoton ionization as a tool of multiple-pulse pump-probe scheme, we demonstrate the modification of the ionization dynamics as we vary the x-ray laser pulse duration. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1301.6459v3-abstract-full').style.display = 'none'; document.getElementById('1301.6459v3-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 6 March, 2013; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 28 January, 2013; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> January 2013. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">9 pages, 4 figures</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Report number:</span> 1301.6459v1 </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> PRL 109, 263001 (2012) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1301.3104">arXiv:1301.3104</a> <span> [<a href="https://arxiv.org/pdf/1301.3104">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> </div> </div> <p class="title is-5 mathjax"> Delayed Ultrafast X-ray Auger Probing (DUXAP) of Nucleobase Ultraviolet Photoprotection </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=McFarland%2C+B+K">B. K. McFarland</a>, <a href="/search/physics?searchtype=author&query=Farrell%2C+J+P">J. P. Farrell</a>, <a href="/search/physics?searchtype=author&query=Miyabe%2C+S">S. Miyabe</a>, <a href="/search/physics?searchtype=author&query=Tarantelli%2C+F">F. Tarantelli</a>, <a href="/search/physics?searchtype=author&query=Aguilar%2C+A">A. Aguilar</a>, <a href="/search/physics?searchtype=author&query=Berrah%2C+N">N. Berrah</a>, <a href="/search/physics?searchtype=author&query=Bostedt%2C+C">C. Bostedt</a>, <a href="/search/physics?searchtype=author&query=Bozek%2C+J">J. Bozek</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">P. H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Castagna%2C+J+C">J. C. Castagna</a>, <a href="/search/physics?searchtype=author&query=Coffee%2C+R">R. Coffee</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J">J. Cryan</a>, <a href="/search/physics?searchtype=author&query=Fang%2C+L">L. Fang</a>, <a href="/search/physics?searchtype=author&query=Feifel%2C+R">R. Feifel</a>, <a href="/search/physics?searchtype=author&query=Gaffney%2C+K">K. Gaffney</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J">J. Glownia</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T">T. Martinez</a>, <a href="/search/physics?searchtype=author&query=Mucke%2C+M">M. Mucke</a>, <a href="/search/physics?searchtype=author&query=Murphy%2C+B">B. Murphy</a>, <a href="/search/physics?searchtype=author&query=Natan%2C+A">A. Natan</a>, <a href="/search/physics?searchtype=author&query=Osipov%2C+T">T. Osipov</a>, <a href="/search/physics?searchtype=author&query=Petrovic%2C+V+.">V . Petrovic</a>, <a href="/search/physics?searchtype=author&query=Schorb%2C+S">S. Schorb</a>, <a href="/search/physics?searchtype=author&query=Schultz%2C+T">Th. Schultz</a>, <a href="/search/physics?searchtype=author&query=Spector%2C+L">L. Spector</a> , et al. (6 additional authors not shown) </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1301.3104v1-abstract-short" style="display: inline;"> We present a new method for ultrafast spectroscopy of molecular photoexcited dynamics. The technique uses a pair of femtosecond pulses: a photoexcitation pulse initiating excited state dynamics followed by a soft x-ray (SXR) probe pulse that core ionizes certain atoms inside the molecule. We observe the Auger decay of the core hole as a function of delay between the photoexcitation and SXR pulses.… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1301.3104v1-abstract-full').style.display = 'inline'; document.getElementById('1301.3104v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1301.3104v1-abstract-full" style="display: none;"> We present a new method for ultrafast spectroscopy of molecular photoexcited dynamics. The technique uses a pair of femtosecond pulses: a photoexcitation pulse initiating excited state dynamics followed by a soft x-ray (SXR) probe pulse that core ionizes certain atoms inside the molecule. We observe the Auger decay of the core hole as a function of delay between the photoexcitation and SXR pulses. The core hole decay is particularly sensitive to the local valence electrons near the core and shows new types of propensity rules, compared to dipole selection rules in SXR absorption or emission spectroscopy. We apply the delayed ultrafast x-ray Auger probing (DUXAP) method to the specific problem of nucleobase photoprotection to demonstrate its potential. The ultraviolet photoexcited 蟺蟺* states of nucleobases are prone to chemical reactions with neighboring bases. To avoid this, the single molecules funnel the 蟺蟺* population to lower lying electronic states on an ultrafast timescale under violation of the Born-Oppenheimer approximation. The new type of propensity rule, which is confirmed by Auger decay simulations, allows us to have increased sensitivity on the direct relaxation from the 蟺蟺* state to the vibrationally hot electronic ground state. For the nucleobase thymine, we measure a decay constant of 300 fs in agreement with previous quantum chemical simulations. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1301.3104v1-abstract-full').style.display = 'none'; document.getElementById('1301.3104v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 14 January, 2013; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> January 2013. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1212.3728">arXiv:1212.3728</a> <span> [<a href="https://arxiv.org/pdf/1212.3728">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Atomic and Molecular Clusters">physics.atm-clus</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1063/1.4829766">10.1063/1.4829766 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Enhancement of strong-field multiple ionization in the vicinity of the conical intersection in 1,3-cyclohexadiene ring opening </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Petrovic%2C+V+S">Vladimir S. Petrovic</a>, <a href="/search/physics?searchtype=author&query=Schorb%2C+S">Sebastian Schorb</a>, <a href="/search/physics?searchtype=author&query=Kim%2C+J">Jaehee Kim</a>, <a href="/search/physics?searchtype=author&query=White%2C+J">James White</a>, <a href="/search/physics?searchtype=author&query=Cryan%2C+J+P">James P. Cryan</a>, <a href="/search/physics?searchtype=author&query=Glownia%2C+J+M">J. Michael Glownia</a>, <a href="/search/physics?searchtype=author&query=Zipp%2C+L">Lucas Zipp</a>, <a href="/search/physics?searchtype=author&query=Broege%2C+D">Douglas Broege</a>, <a href="/search/physics?searchtype=author&query=Miyabe%2C+S">Shungo Miyabe</a>, <a href="/search/physics?searchtype=author&query=Tao%2C+H">Hongli Tao</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T">Todd Martinez</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1212.3728v3-abstract-short" style="display: inline;"> Nonradiative energy dissipation in electronically excited polyatomic molecules proceeds through conical intersections, loci of degeneracy between electronic states. We observe a marked enhancement of laser-induced double ionization in the vicinity of a conical intersection during a non-radiative transition. We measured double ionization by detecting the kinetic energy of ions released by laser-ind… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1212.3728v3-abstract-full').style.display = 'inline'; document.getElementById('1212.3728v3-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1212.3728v3-abstract-full" style="display: none;"> Nonradiative energy dissipation in electronically excited polyatomic molecules proceeds through conical intersections, loci of degeneracy between electronic states. We observe a marked enhancement of laser-induced double ionization in the vicinity of a conical intersection during a non-radiative transition. We measured double ionization by detecting the kinetic energy of ions released by laser-induced strong-field fragmentation during the ring-opening transition between 1,3-cyclohexadiene and 1,3,5-hexatriene. The enhancement of the double ionization correlates with the conical intersection between the HOMO and LUMO orbitals. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1212.3728v3-abstract-full').style.display = 'none'; document.getElementById('1212.3728v3-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 8 November, 2013; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 15 December, 2012; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> December 2012. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">The manuscript has been accepted for publication at the Journal of Chemical Physics (October 28 2013)</span> </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1207.2517">arXiv:1207.2517</a> <span> [<a href="https://arxiv.org/pdf/1207.2517">pdf</a>, <a href="https://arxiv.org/format/1207.2517">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1038/ncomms4190">10.1038/ncomms4190 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Orientational decomposition of molecular high harmonic emission in three dimensions </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Spector%2C+L+S">Limor S. Spector</a>, <a href="/search/physics?searchtype=author&query=Artamonov%2C+M">Maxim Artamonov</a>, <a href="/search/physics?searchtype=author&query=Miyabe%2C+S">Shungo Miyabe</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T">Todd Martinez</a>, <a href="/search/physics?searchtype=author&query=Seideman%2C+T">Tamar Seideman</a>, <a href="/search/physics?searchtype=author&query=Guehr%2C+M">Markus Guehr</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1207.2517v2-abstract-short" style="display: inline;"> An important goal in molecular physics and chemistry today is to obtain structure-dependent information about molecular function to obtain a deeper understanding into chemical reactions. However, until now, asymmetric tops, which comprise the widest and most general class of molecules, remain principally unexplored. This gap is particularly evident in high harmonic generation (HHG). HHG has succes… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1207.2517v2-abstract-full').style.display = 'inline'; document.getElementById('1207.2517v2-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1207.2517v2-abstract-full" style="display: none;"> An important goal in molecular physics and chemistry today is to obtain structure-dependent information about molecular function to obtain a deeper understanding into chemical reactions. However, until now, asymmetric tops, which comprise the widest and most general class of molecules, remain principally unexplored. This gap is particularly evident in high harmonic generation (HHG). HHG has successfully obtained structural information about electron hole pairs or orbitals for simple linear molecules. Unfortunately, for more complicated molecules, the emission from different molecular directions interfere, concealing individual angular signatures. Here we introduce a method to extract orientation-dependent information from asymmetric tops and apply it to the sulfur dioxide (SO2) molecule. We use the rotational revival structure to decompose the angular contributions of HHG emission. This method also extends HHG-based tomographic imaging into three dimensions and makes it applicable to a much wider class of systems than previously envisioned. Our results suggest that HHG is a powerful tool to probe electron orbital structure and dynamics of complex molecules. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1207.2517v2-abstract-full').style.display = 'none'; document.getElementById('1207.2517v2-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 18 January, 2013; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 10 July, 2012; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> July 2012. </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Comments:</span> <span class="has-text-grey-dark mathjax">Main text and supplementary information</span> </p> <p class="comments is-size-7"> <span class="has-text-black-bis has-text-weight-semibold">Journal ref:</span> Nat, Communications 5, 3190 (2014) </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1109.5756">arXiv:1109.5756</a> <span> [<a href="https://arxiv.org/pdf/1109.5756">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1021/jp208384b">10.1021/jp208384b <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Control of 1,3-Cyclohexadiene Photoisomerization Using Light-Induced Conical Intersections </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Kim%2C+J">Jaehee Kim</a>, <a href="/search/physics?searchtype=author&query=Tao%2C+H">Hongli Tao</a>, <a href="/search/physics?searchtype=author&query=White%2C+J+L">James L. White</a>, <a href="/search/physics?searchtype=author&query=Petrovic%2C+V+S">Vladimir S. Petrovic</a>, <a href="/search/physics?searchtype=author&query=Martinez%2C+T+J">Todd J. Martinez</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1109.5756v3-abstract-short" style="display: inline;"> We have studied the photo-induced isomerization from 1,3-cyclohexadiene to 1,3,5-hexatriene in the presence of an intense ultrafast laser pulse. We find that the laser field maximally suppresses isomerization if it is both polarized parallel to the excitation dipole and present 50 fs after the initial photoabsorption, at the time when the system is expected to be in the vicinity of a conical inter… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1109.5756v3-abstract-full').style.display = 'inline'; document.getElementById('1109.5756v3-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1109.5756v3-abstract-full" style="display: none;"> We have studied the photo-induced isomerization from 1,3-cyclohexadiene to 1,3,5-hexatriene in the presence of an intense ultrafast laser pulse. We find that the laser field maximally suppresses isomerization if it is both polarized parallel to the excitation dipole and present 50 fs after the initial photoabsorption, at the time when the system is expected to be in the vicinity of a conical intersection that mediates this structural transition. A modified ab initio multiple spawning (AIMS) method shows that the laser induces a resonant coupling between the excited state and the ground state, i.e., a light-induced conical intersection. The theory accounts for the timing and direction of the effect. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1109.5756v3-abstract-full').style.display = 'none'; document.getElementById('1109.5756v3-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 8 November, 2011; <span class="has-text-black-bis has-text-weight-semibold">v1</span> submitted 26 September, 2011; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> September 2011. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1109.2702">arXiv:1109.2702</a> <span> [<a href="https://arxiv.org/pdf/1109.2702">pdf</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Chemical Physics">physics.chem-ph</span> <span class="tag is-small is-grey tooltip is-tooltip-top" data-tooltip="Quantum Physics">quant-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1063/1.3681258">10.1063/1.3681258 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Ultrafast ring opening in CHD investigated by simplex-based spectral unmixing </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=White%2C+J+L">James L. White</a>, <a href="/search/physics?searchtype=author&query=Kim%2C+J">Jaehee Kim</a>, <a href="/search/physics?searchtype=author&query=Petrovic%2C+V+S">Vladimir S. Petrovic</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1109.2702v1-abstract-short" style="display: inline;"> We use spectral unmixing to determine the number of transient photoproducts and to track their evolution following the photo- excitation of 1,3-cyclohexadiene (CHD) to form 1,3,5-hexatriene (HT) in the gas phase. The ring opening is initiated with a 266 nm ultraviolet laser pulse and probed via fragmentation with a delayed intense infrared 800 nm laser pulse. The ion time-of-flight (TOF) spectra a… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1109.2702v1-abstract-full').style.display = 'inline'; document.getElementById('1109.2702v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1109.2702v1-abstract-full" style="display: none;"> We use spectral unmixing to determine the number of transient photoproducts and to track their evolution following the photo- excitation of 1,3-cyclohexadiene (CHD) to form 1,3,5-hexatriene (HT) in the gas phase. The ring opening is initiated with a 266 nm ultraviolet laser pulse and probed via fragmentation with a delayed intense infrared 800 nm laser pulse. The ion time-of-flight (TOF) spectra are analyzed with a simplex-based spectral unmixing technique. We find that at least three independent spectra are needed to model the transient TOF spectra. Guided by mathematical and physical constraints, we decompose the transient TOF spectra into three spectra associated with the presence of CHD, CHD+, and HT, and show how these three products appear at different times during the ring opening. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1109.2702v1-abstract-full').style.display = 'none'; document.getElementById('1109.2702v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 13 September, 2011; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> September 2011. </p> </li> <li class="arxiv-result"> <div class="is-marginless"> <p class="list-title is-inline-block"><a href="https://arxiv.org/abs/1103.4423">arXiv:1103.4423</a> <span> [<a href="https://arxiv.org/pdf/1103.4423">pdf</a>, <a href="https://arxiv.org/format/1103.4423">other</a>] </span> </p> <div class="tags is-inline-block"> <span class="tag is-small is-link tooltip is-tooltip-top" data-tooltip="Atomic Physics">physics.atom-ph</span> </div> <div class="is-inline-block" style="margin-left: 0.5rem"> <div class="tags has-addons"> <span class="tag is-dark is-size-7">doi</span> <span class="tag is-light is-size-7"><a class="" href="https://doi.org/10.1103/PhysRevLett.107.083001">10.1103/PhysRevLett.107.083001 <i class="fa fa-external-link" aria-hidden="true"></i></a></span> </div> </div> </div> <p class="title is-5 mathjax"> Strong field ionization to multiple electronic states in water </p> <p class="authors"> <span class="search-hit">Authors:</span> <a href="/search/physics?searchtype=author&query=Farrell%2C+J+P">Joe P. Farrell</a>, <a href="/search/physics?searchtype=author&query=Petretti%2C+S">Simon Petretti</a>, <a href="/search/physics?searchtype=author&query=F%C3%B6rster%2C+J">Johann F枚rster</a>, <a href="/search/physics?searchtype=author&query=McFarland%2C+B+K">Brian K. McFarland</a>, <a href="/search/physics?searchtype=author&query=Spector%2C+L+S">Limor S. Spector</a>, <a href="/search/physics?searchtype=author&query=Vanne%2C+Y+V">Yulian V. Vanne</a>, <a href="/search/physics?searchtype=author&query=Decleva%2C+P">Piero Decleva</a>, <a href="/search/physics?searchtype=author&query=Bucksbaum%2C+P+H">Philip H. Bucksbaum</a>, <a href="/search/physics?searchtype=author&query=Saenz%2C+A">Alejandro Saenz</a>, <a href="/search/physics?searchtype=author&query=G%C3%BChr%2C+M">Markus G眉hr</a> </p> <p class="abstract mathjax"> <span class="has-text-black-bis has-text-weight-semibold">Abstract</span>: <span class="abstract-short has-text-grey-dark mathjax" id="1103.4423v1-abstract-short" style="display: inline;"> High harmonic spectra show that laser-induced strong field ionization of water has a significant contribution from an inner-valence orbital. Our experiment uses the ratio of H2O and D2O high harmonic yields to isolate the characteristic nuclear motion of the molecular ionic states. The nuclear motion initiated via ionization of the highest occupied molecular orbital (HOMO) is small and is expected… <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1103.4423v1-abstract-full').style.display = 'inline'; document.getElementById('1103.4423v1-abstract-short').style.display = 'none';">▽ More</a> </span> <span class="abstract-full has-text-grey-dark mathjax" id="1103.4423v1-abstract-full" style="display: none;"> High harmonic spectra show that laser-induced strong field ionization of water has a significant contribution from an inner-valence orbital. Our experiment uses the ratio of H2O and D2O high harmonic yields to isolate the characteristic nuclear motion of the molecular ionic states. The nuclear motion initiated via ionization of the highest occupied molecular orbital (HOMO) is small and is expected to lead to similar harmonic yields for the two isotopes. In contrast, ionization of the second least bound orbital (HOMO-1) exhibits itself via a strong bending motion which creates a significant isotope effect. We elaborate on this interpretation by simulating strong field ionization and high harmonic generation from the water isotopes using the time-dependent Schr枚dinger equation. We expect that this isotope marking scheme for probing excited ionic states in strong field processes can be generalized to other molecules. <a class="is-size-7" style="white-space: nowrap;" onclick="document.getElementById('1103.4423v1-abstract-full').style.display = 'none'; document.getElementById('1103.4423v1-abstract-short').style.display = 'inline';">△ Less</a> </span> </p> <p class="is-size-7"><span class="has-text-black-bis has-text-weight-semibold">Submitted</span> 22 March, 2011; <span class="has-text-black-bis has-text-weight-semibold">originally announced</span> March 2011. </p> </li> </ol> <nav class="pagination is-small is-centered breathe-horizontal" role="navigation" aria-label="pagination"> <a href="" class="pagination-previous is-invisible">Previous </a> <a href="/search/?searchtype=author&query=Bucksbaum%2C+P+H&start=50" class="pagination-next" >Next </a> <ul class="pagination-list"> <li> <a href="/search/?searchtype=author&query=Bucksbaum%2C+P+H&start=0" 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