[2411.01700] Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule

<?xml version="1.0" encoding="UTF-8"?> <!DOCTYPE html PUBLIC "-//W3C//DTD XHTML 1.0 Transitional//EN" "http://www.w3.org/TR/xhtml1/DTD/xhtml1-transitional.dtd"> <html xmlns="http://www.w3.org/1999/xhtml" lang="en" xml:lang="en"> <head> <title>[2411.01700] Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule</title> <meta name="viewport" content="width=device-width, initial-scale=1"> <link rel="apple-touch-icon" sizes="180x180" href="/static/browse/0.3.4/images/icons/apple-touch-icon.png"> <link rel="icon" type="image/png" sizes="32x32" href="/static/browse/0.3.4/images/icons/favicon-32x32.png"> <link rel="icon" type="image/png" sizes="16x16" href="/static/browse/0.3.4/images/icons/favicon-16x16.png"> <link rel="manifest" href="/static/browse/0.3.4/images/icons/site.webmanifest"> <link rel="mask-icon" href="/static/browse/0.3.4/images/icons/safari-pinned-tab.svg" color="#5bbad5"> <meta name="msapplication-TileColor" content="#da532c"> <meta name="theme-color" content="#ffffff"> <link rel="stylesheet" type="text/css" media="screen" href="/static/browse/0.3.4/css/arXiv.css?v=20240822" /> <link rel="stylesheet" type="text/css" media="print" href="/static/browse/0.3.4/css/arXiv-print.css?v=20200611" /> <link rel="stylesheet" type="text/css" media="screen" href="/static/browse/0.3.4/css/browse_search.css" /> <script language="javascript" src="/static/browse/0.3.4/js/accordion.js" /></script> <link rel="canonical" href="https://arxiv.org/abs/2411.01700"/> <meta name="description" content="Abstract page for arXiv paper 2411.01700: Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule"><meta property="og:type" content="website" /> <meta property="og:site_name" content="arXiv.org" /> <meta property="og:title" content="Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule" /> <meta property="og:url" content="https://arxiv.org/abs/2411.01700v1" /> <meta property="og:image" content="/static/browse/0.3.4/images/arxiv-logo-fb.png" /> <meta property="og:image:secure_url" content="/static/browse/0.3.4/images/arxiv-logo-fb.png" /> <meta property="og:image:width" content="1200" /> <meta property="og:image:height" content="700" /> <meta property="og:image:alt" content="arXiv logo"/> <meta property="og:description" content="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."/> <meta name="twitter:site" content="@arxiv"/> <meta name="twitter:card" content="summary"/> <meta name="twitter:title" content="Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule"/> <meta name="twitter:description" content="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..."/> <meta name="twitter:image" content="https://static.arxiv.org/icons/twitter/arxiv-logo-twitter-square.png"/> <meta name="twitter:image:alt" content="arXiv logo"/> <link rel="stylesheet" media="screen" type="text/css" href="/static/browse/0.3.4/css/tooltip.css"/><link rel="stylesheet" media="screen" type="text/css" href="https://static.arxiv.org/js/bibex-dev/bibex.css?20200709"/> <script src="/static/browse/0.3.4/js/mathjaxToggle.min.js" type="text/javascript"></script> <script src="//code.jquery.com/jquery-latest.min.js" type="text/javascript"></script> <script src="//cdn.jsdelivr.net/npm/js-cookie@2/src/js.cookie.min.js" type="text/javascript"></script> <script src="//cdn.jsdelivr.net/npm/dompurify@2.3.5/dist/purify.min.js"></script> <script src="/static/browse/0.3.4/js/toggle-labs.js?20241022" type="text/javascript"></script> <script src="/static/browse/0.3.4/js/cite.js" type="text/javascript"></script><meta name="citation_title" content="Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule" /><meta name="citation_author" content="Driver, Taran" /><meta name="citation_author" content="Guo, Zhaoheng" /><meta name="citation_author" content="Isele, Erik" /><meta name="citation_author" content="Grell, Gilbert" /><meta name="citation_author" content="Ruberti, Marco" /><meta name="citation_author" content="ONeal, Jordan T." /><meta name="citation_author" content="Alexander, Oliver" /><meta name="citation_author" content="Beauvarlet, Sandra" /><meta name="citation_author" content="Cesar, David" /><meta name="citation_author" content="Duris, Joseph" /><meta name="citation_author" content="Garratt, Douglas" /><meta name="citation_author" content="Larsen, Kirk A." /><meta name="citation_author" content="Li, Siqi" /><meta name="citation_author" content="Koloren膷, P艡emysl" /><meta name="citation_author" content="McCracken, Gregory A." /><meta name="citation_author" content="Tuthill, Daniel" /><meta name="citation_author" content="Wang, Zifan" /><meta name="citation_author" content="Berrah, Nora" /><meta name="citation_author" content="Bostedt, Christoph" /><meta name="citation_author" content="Borne, Kurtis" /><meta name="citation_author" content="Cheng, Xinxin" /><meta name="citation_author" content="DiMauro, Louis F." /><meta name="citation_author" content="Doumy, Gilles" /><meta name="citation_author" content="Franz, Paris L." /><meta name="citation_author" content="Kamalov, Andrei" /><meta name="citation_author" content="Li, Xiang" /><meta name="citation_author" content="Lin, Ming-Fu" /><meta name="citation_author" content="Obaid, Razib" /><meta name="citation_author" content="Pic贸n, Antonio" /><meta name="citation_author" content="Robles, River R." /><meta name="citation_author" content="Rolles, Daniel" /><meta name="citation_author" content="Rudenko, Artem" /><meta name="citation_author" content="Shaikh, Moniruzzaman" /><meta name="citation_author" content="Slaughter, Daniel S." /><meta name="citation_author" content="Sudar, Nicholas S." /><meta name="citation_author" content="Thierstein, Emily" /><meta name="citation_author" content="Ueda, Kiyoshi" /><meta name="citation_author" content="Wang, Enliang" /><meta name="citation_author" content="Wang, Anna L." /><meta name="citation_author" content="Weber, Thorsten" /><meta name="citation_author" content="Wolf, Thomas J. A." /><meta name="citation_author" content="Young, Linda" /><meta name="citation_author" content="Zhang, Zhen" /><meta name="citation_author" content="Averbukh, Vitali" /><meta name="citation_author" content="Gessner, Oliver" /><meta name="citation_author" content="Bucksbaum, Philip H." /><meta name="citation_author" content="Kling, Matthias F." /><meta name="citation_author" content="Palacios, Alicia" /><meta name="citation_author" content="Mart铆n, Fernando" /><meta name="citation_author" content="Marangos, Jon P." /><meta name="citation_author" content="Walter, Peter" /><meta name="citation_author" content="Marinelli, Agostino" /><meta name="citation_author" content="Cryan, James P." /><meta name="citation_date" content="2024/11/03" /><meta name="citation_online_date" content="2024/11/03" /><meta name="citation_pdf_url" content="http://arxiv.org/pdf/2411.01700" /><meta name="citation_arxiv_id" content="2411.01700" /><meta name="citation_abstract" content="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." /> </head> <body class="with-cu-identity"> <div class="flex-wrap-footer"> <header> <a href="#content" class="is-sr-only">Skip to main content</a>  <div class="columns is-vcentered is-hidden-mobile" id="cu-identity"> <div class="column" id="cu-logo"> <a href="https://www.cornell.edu/"><img src="/static/browse/0.3.4/images/icons/cu/cornell-reduced-white-SMALL.svg" alt="Cornell University" /></a> </div><div class="column" id="support-ack"> <span id="support-ack-url">We gratefully acknowledge support from the Simons Foundation, <a href="https://info.arxiv.org/about/ourmembers.html">member institutions</a>, and all contributors.</span> <a href="https://info.arxiv.org/about/donate.html" class="btn-header-donate">Donate</a> </div> </div> <div id="header" 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href="https://arxiv.org/search/physics?searchtype=author&query=Driver,+T" rel="nofollow">Taran Driver</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Guo,+Z" rel="nofollow">Zhaoheng Guo</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Isele,+E" rel="nofollow">Erik Isele</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Grell,+G" rel="nofollow">Gilbert Grell</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Ruberti,+M" rel="nofollow">Marco Ruberti</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=ONeal,+J+T" rel="nofollow">Jordan T. ONeal</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Alexander,+O" rel="nofollow">Oliver Alexander</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Beauvarlet,+S" rel="nofollow">Sandra Beauvarlet</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Cesar,+D" rel="nofollow">David Cesar</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Duris,+J" rel="nofollow">Joseph Duris</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Garratt,+D" rel="nofollow">Douglas Garratt</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Larsen,+K+A" rel="nofollow">Kirk A. Larsen</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Li,+S" rel="nofollow">Siqi Li</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Koloren%C4%8D,+P" rel="nofollow">P艡emysl Koloren膷</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=McCracken,+G+A" rel="nofollow">Gregory A. McCracken</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Tuthill,+D" rel="nofollow">Daniel Tuthill</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Wang,+Z" rel="nofollow">Zifan Wang</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Berrah,+N" rel="nofollow">Nora Berrah</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Bostedt,+C" rel="nofollow">Christoph Bostedt</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Borne,+K" rel="nofollow">Kurtis Borne</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Cheng,+X" rel="nofollow">Xinxin Cheng</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=DiMauro,+L+F" rel="nofollow">Louis F. DiMauro</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Doumy,+G" rel="nofollow">Gilles Doumy</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Franz,+P+L" rel="nofollow">Paris L. Franz</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Kamalov,+A" rel="nofollow">Andrei Kamalov</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Li,+X" rel="nofollow">Xiang Li</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Lin,+M" rel="nofollow">Ming-Fu Lin</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Obaid,+R" rel="nofollow">Razib Obaid</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Pic%C3%B3n,+A" rel="nofollow">Antonio Pic贸n</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Robles,+R+R" rel="nofollow">River R. Robles</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Rolles,+D" rel="nofollow">Daniel Rolles</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Rudenko,+A" rel="nofollow">Artem Rudenko</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Shaikh,+M" rel="nofollow">Moniruzzaman Shaikh</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Slaughter,+D+S" rel="nofollow">Daniel S. Slaughter</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Sudar,+N+S" rel="nofollow">Nicholas S. Sudar</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Thierstein,+E" rel="nofollow">Emily Thierstein</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Ueda,+K" rel="nofollow">Kiyoshi Ueda</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Wang,+E" rel="nofollow">Enliang Wang</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Wang,+A+L" rel="nofollow">Anna L. Wang</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Weber,+T" rel="nofollow">Thorsten Weber</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Wolf,+T+J+A" rel="nofollow">Thomas J. A. Wolf</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Young,+L" rel="nofollow">Linda Young</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Zhang,+Z" rel="nofollow">Zhen Zhang</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Averbukh,+V" rel="nofollow">Vitali Averbukh</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Gessner,+O" rel="nofollow">Oliver Gessner</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Bucksbaum,+P+H" rel="nofollow">Philip H. Bucksbaum</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Kling,+M+F" rel="nofollow">Matthias F. Kling</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Palacios,+A" rel="nofollow">Alicia Palacios</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Mart%C3%ADn,+F" rel="nofollow">Fernando Mart铆n</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Marangos,+J+P" rel="nofollow">Jon P. Marangos</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Walter,+P" rel="nofollow">Peter Walter</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Marinelli,+A" rel="nofollow">Agostino Marinelli</a>, <a href="https://arxiv.org/search/physics?searchtype=author&query=Cryan,+J+P" rel="nofollow">James P. Cryan</a></div> <div id="download-button-info" hidden>View a PDF of the paper titled Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule, by Taran Driver and 51 other authors</div> <a class="mobile-submission-download" href="/pdf/2411.01700">View PDF</a> <a class="mobile-submission-download" href="https://arxiv.org/html/2411.01700v1">HTML (experimental)</a> <blockquote class="abstract mathjax"> <span class="descriptor">Abstract:</span>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. </blockquote>  <div class="metatable"> <table summary="Additional metadata"><tr> <td class="tablecell label">Subjects:</td> <td class="tablecell subjects"> <span class="primary-subject">Chemical Physics (physics.chem-ph)</span></td> </tr><tr> <td class="tablecell label">Cite as:</td> <td class="tablecell arxivid"><span class="arxivid"><a href="https://arxiv.org/abs/2411.01700">arXiv:2411.01700</a> [physics.chem-ph]</span></td> </tr> <tr> <td class="tablecell label"> </td> <td class="tablecell arxividv">(or <span class="arxivid"> <a href="https://arxiv.org/abs/2411.01700v1">arXiv:2411.01700v1</a> [physics.chem-ph]</span> for this version) </td> </tr> <tr> <td class="tablecell label"> </td> <td class="tablecell arxivdoi"> <a href="https://doi.org/10.48550/arXiv.2411.01700" id="arxiv-doi-link">https://doi.org/10.48550/arXiv.2411.01700</a><div class="button-and-tooltip"> <button class="more-info" aria-describedby="more-info-desc-1"> <svg height="15" role="presentation" xmlns="http://www.w3.org/2000/svg" viewBox="0 0 512 512"><path fill="currentColor" d="M256 8C119.043 8 8 119.083 8 256c0 136.997 111.043 248 248 248s248-111.003 248-248C504 119.083 392.957 8 256 8zm0 110c23.196 0 42 18.804 42 42s-18.804 42-42 42-42-18.804-42-42 18.804-42 42-42zm56 254c0 6.627-5.373 12-12 12h-88c-6.627 0-12-5.373-12-12v-24c0-6.627 5.373-12 12-12h12v-64h-12c-6.627 0-12-5.373-12-12v-24c0-6.627 5.373-12 12-12h64c6.627 0 12 5.373 12 12v100h12c6.627 0 12 5.373 12 12v24z" class=""></path></svg> <span class="visually-hidden">Focus to learn more</span> </button>  <div role="tooltip" id="more-info-desc-1"> <span class="left-corner"></span> arXiv-issued DOI via DataCite</div> </div> </td> </tr></table> </div> </div> </div> <div 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[2411.01700] Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule