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Controlling attosecond electron dynamics by phase-stabilized polarization gating | Nature Physics

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When the laser field drives the wavepackets back to the parent ion, they interfere with the bound wavefunction, producing coherent subfemtosecond extreme-ultraviolet light bursts. When only a single return is possible2,3, an isolated attosecond pulse is generated. Here we demonstrate that by modulating the polarization of a carrier-envelope phase-stabilized short laser pulse4, we can finely control the electron-wavepacket dynamics. We use high-order harmonic generation to probe these dynamics. Under optimized conditions, we observe the signature of a single return of the electron wavepacket over a large range of energies. This temporally confines the extreme-ultraviolet emission to an isolated attosecond pulse with a broad and tunable bandwidth. Our approach is very general, and extends the bandwidth of attosecond isolated pulses in such a way that pulses of a few attoseconds seem achievable. Similar temporal resolution could also be achieved by directly using the broadband electron wavepacket. 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J.">I. J. Sola</a><sup class="u-js-hide"><a href="#Aff1">1</a></sup>, </li><li class="c-article-author-list__item"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-E_-M_vel-Aff1" data-author-popup="auth-E_-M_vel-Aff1" data-author-search="Mével, E.">E. Mével</a><sup class="u-js-hide"><a href="#Aff1">1</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-L_-Elouga-Aff1" data-author-popup="auth-L_-Elouga-Aff1" data-author-search="Elouga, L.">L. Elouga</a><sup class="u-js-hide"><a href="#Aff1">1</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-E_-Constant-Aff1" data-author-popup="auth-E_-Constant-Aff1" data-author-search="Constant, E." data-corresp-id="c1">E. Constant<svg width="16" height="16" focusable="false" role="img" aria-hidden="true" class="u-icon"><use xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="#icon-eds-i-mail-medium"></use></svg></a><sup class="u-js-hide"><a href="#Aff1">1</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-V_-Strelkov-Aff2" data-author-popup="auth-V_-Strelkov-Aff2" data-author-search="Strelkov, V.">V. Strelkov</a><sup class="u-js-hide"><a href="#Aff2">2</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-L_-Poletto-Aff3" data-author-popup="auth-L_-Poletto-Aff3" data-author-search="Poletto, L.">L. Poletto</a><sup class="u-js-hide"><a href="#Aff3">3</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-P_-Villoresi-Aff3" data-author-popup="auth-P_-Villoresi-Aff3" data-author-search="Villoresi, P.">P. Villoresi</a><sup class="u-js-hide"><a href="#Aff3">3</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-E_-Benedetti-Aff4" data-author-popup="auth-E_-Benedetti-Aff4" data-author-search="Benedetti, E.">E. Benedetti</a><sup class="u-js-hide"><a href="#Aff4">4</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-J__P_-Caumes-Aff4" data-author-popup="auth-J__P_-Caumes-Aff4" data-author-search="Caumes, J.-P.">J.-P. Caumes</a><sup class="u-js-hide"><a href="#Aff4">4</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-S_-Stagira-Aff4" data-author-popup="auth-S_-Stagira-Aff4" data-author-search="Stagira, S.">S. Stagira</a><sup class="u-js-hide"><a href="#Aff4">4</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-C_-Vozzi-Aff4" data-author-popup="auth-C_-Vozzi-Aff4" data-author-search="Vozzi, C.">C. Vozzi</a><sup class="u-js-hide"><a href="#Aff4">4</a></sup>, </li><li class="c-article-author-list__item c-article-author-list__item--hide-small-screen"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-G_-Sansone-Aff4" data-author-popup="auth-G_-Sansone-Aff4" data-author-search="Sansone, G.">G. Sansone</a><sup class="u-js-hide"><a href="#Aff4">4</a></sup> &amp; </li><li class="c-article-author-list__show-more" aria-label="Show all 13 authors for this article" title="Show all 13 authors for this article">…</li><li class="c-article-author-list__item"><a data-test="author-name" data-track="click" data-track-action="open author" data-track-label="link" href="#auth-M_-Nisoli-Aff4" data-author-popup="auth-M_-Nisoli-Aff4" data-author-search="Nisoli, M.">M. Nisoli</a><sup class="u-js-hide"><a href="#Aff4">4</a></sup> </li></ul><button aria-expanded="false" class="c-article-author-list__button"><svg width="16" height="16" focusable="false" role="img" aria-hidden="true" class="u-icon"><use xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="#icon-eds-i-chevron-down-medium"></use></svg><span>Show authors</span></button> <p class="c-article-info-details" data-container-section="info"> <a data-test="journal-link" href="/nphys" data-track="click" data-track-action="journal homepage" data-track-category="article body" data-track-label="link"><i data-test="journal-title">Nature Physics</i></a> <b data-test="journal-volume"><span class="u-visually-hidden">volume</span> 2</b>, <span class="u-visually-hidden">pages </span>319–322 (<span data-test="article-publication-year">2006</span>)<a href="#citeas" class="c-article-info-details__cite-as u-hide-print" data-track="click" data-track-action="cite this article" data-track-label="link">Cite this article</a> </p> <div class="c-article-metrics-bar__wrapper u-clear-both"> <ul class="c-article-metrics-bar u-list-reset"> <li class=" c-article-metrics-bar__item" data-test="access-count"> <p class="c-article-metrics-bar__count">5095 <span class="c-article-metrics-bar__label">Accesses</span></p> </li> <li class="c-article-metrics-bar__item" data-test="citation-count"> <p class="c-article-metrics-bar__count">385 <span class="c-article-metrics-bar__label">Citations</span></p> </li> <li class="c-article-metrics-bar__item"> <p class="c-article-metrics-bar__details"><a href="/articles/nphys281/metrics" data-track="click" data-track-action="view metrics" data-track-label="link" rel="nofollow">Metrics <span class="u-visually-hidden">details</span></a></p> </li> </ul> </div> </header> </div> <div class="c-article-body"> <section aria-labelledby="Abs1" data-title="Abstract" lang="en"><div class="c-article-section" id="Abs1-section"><h2 class="c-article-section__title js-section-title js-c-reading-companion-sections-item" id="Abs1">Abstract</h2><div class="c-article-section__content" id="Abs1-content"><p>Attosecond electron wavepackets are produced when an intense laser field ionizes an atom or a molecule<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 1" title="Corkum, P. B. Plasma perspective on strong-field multiphoton ionization. Phys. Rev. Lett. 71, 1994–1997 (1993)." href="/articles/nphys281#ref-CR1" id="ref-link-section-d25713248e485">1</a></sup>. When the laser field drives the wavepackets back to the parent ion, they interfere with the bound wavefunction, producing coherent subfemtosecond extreme-ultraviolet light bursts. When only a single return is possible<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 2" title="Corkum, P. B., Burnett, N. H. &amp; Ivanov, M. Y. Subfemtosecond pulses. Opt. Lett. 19, 1870–1872 (1994)." href="/articles/nphys281#ref-CR2" id="ref-link-section-d25713248e489">2</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 3" title="Christov, I. P., Murnane, M. M. &amp; Kapteyn, H. C. High-harmonic generation of attosecond pulses in the single-cycle regime. Phys. Rev. Lett. 78, 1251–1254 (1997)." href="/articles/nphys281#ref-CR3" id="ref-link-section-d25713248e492">3</a></sup>, an isolated attosecond pulse is generated. Here we demonstrate that by modulating the polarization of a carrier-envelope phase-stabilized short laser pulse<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 4" title="Baltuška, A. et al. Attosecond control of electronic process by intense light fields. Nature 421, 611–615 (2003)." href="/articles/nphys281#ref-CR4" id="ref-link-section-d25713248e496">4</a></sup>, we can finely control the electron-wavepacket dynamics. We use high-order harmonic generation to probe these dynamics. Under optimized conditions, we observe the signature of a single return of the electron wavepacket over a large range of energies. This temporally confines the extreme-ultraviolet emission to an isolated attosecond pulse with a broad and tunable bandwidth. Our approach is very general, and extends the bandwidth of attosecond isolated pulses in such a way that pulses of a few attoseconds seem achievable. Similar temporal resolution could also be achieved by directly using the broadband electron wavepacket. This opens up a new regime for time-resolved tomography of atomic or molecular wavefunctions<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 5" title="Itatani, J. et al. Tomographic imaging of molecular orbitals. Nature 432, 867–871 (2004)." href="/articles/nphys281#ref-CR5" id="ref-link-section-d25713248e500">5</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 6" title="Nikura, H., Villeneuve, D. M. &amp; Corkum, P. B. Mapping attosecond electron wave packet motion. Phys. Rev. Lett. 94, 083003 (2005)." href="/articles/nphys281#ref-CR6" id="ref-link-section-d25713248e503">6</a></sup> and ultrafast dynamics.</p></div></div></section> <noscript> </noscript> <section aria-labelledby="inline-recommendations" data-title="Inline Recommendations" class="c-article-recommendations" data-track-component="inline-recommendations"> <h3 class="c-article-recommendations-title" id="inline-recommendations">Similar content being viewed by others</h3> <div class="c-article-recommendations-list"> <div class="c-article-recommendations-list__item"> <article class="c-article-recommendations-card" itemscope itemtype="http://schema.org/ScholarlyArticle"> <div class="c-article-recommendations-card__img"><img src="https://media.springernature.com/w215h120/springer-static/image/art%3A10.1038%2Fs41467-021-26772-0/MediaObjects/41467_2021_26772_Fig1_HTML.png" loading="lazy" alt=""></div> <div class="c-article-recommendations-card__main"> <h3 class="c-article-recommendations-card__heading" itemprop="name headline"> <a class="c-article-recommendations-card__link" itemprop="url" href="https://www.nature.com/articles/s41467-021-26772-0?fromPaywallRec=false" data-track="select_recommendations_1" data-track-context="inline recommendations" data-track-action="click recommendations inline - 1" data-track-label="10.1038/s41467-021-26772-0">Strong-field coherent control of isolated attosecond pulse generation </a> </h3> <div class="c-article-meta-recommendations" data-test="recommendation-info"> <span class="c-article-meta-recommendations__item-type">Article</span> <span class="c-article-meta-recommendations__access-type">Open access</span> <span class="c-article-meta-recommendations__date">17 November 2021</span> </div> </div> </article> </div> <div class="c-article-recommendations-list__item"> <article class="c-article-recommendations-card" itemscope itemtype="http://schema.org/ScholarlyArticle"> <div class="c-article-recommendations-card__img"><img src="https://media.springernature.com/w215h120/springer-static/image/art%3A10.1038%2Fs41586-020-2005-6/MediaObjects/41586_2020_2005_Fig1_HTML.png" loading="lazy" alt=""></div> <div class="c-article-recommendations-card__main"> <h3 class="c-article-recommendations-card__heading" itemprop="name headline"> <a class="c-article-recommendations-card__link" itemprop="url" href="https://www.nature.com/articles/s41586-020-2005-6?fromPaywallRec=false" data-track="select_recommendations_2" data-track-context="inline recommendations" data-track-action="click recommendations inline - 2" data-track-label="10.1038/s41586-020-2005-6">Attosecond pulse shaping using a seeded free-electron laser </a> </h3> <div class="c-article-meta-recommendations" data-test="recommendation-info"> <span class="c-article-meta-recommendations__item-type">Article</span> <span class="c-article-meta-recommendations__date">10 February 2020</span> </div> </div> </article> </div> <div class="c-article-recommendations-list__item"> <article class="c-article-recommendations-card" itemscope itemtype="http://schema.org/ScholarlyArticle"> <div class="c-article-recommendations-card__img"><img src="https://media.springernature.com/w215h120/springer-static/image/art%3A10.1038%2Fs41467-020-14721-2/MediaObjects/41467_2020_14721_Fig1_HTML.png" loading="lazy" alt=""></div> <div class="c-article-recommendations-card__main"> <h3 class="c-article-recommendations-card__heading" itemprop="name headline"> <a class="c-article-recommendations-card__link" itemprop="url" href="https://www.nature.com/articles/s41467-020-14721-2?fromPaywallRec=false" data-track="select_recommendations_3" data-track-context="inline recommendations" data-track-action="click recommendations inline - 3" data-track-label="10.1038/s41467-020-14721-2">Tracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses </a> </h3> <div class="c-article-meta-recommendations" data-test="recommendation-info"> <span class="c-article-meta-recommendations__item-type">Article</span> <span class="c-article-meta-recommendations__access-type">Open access</span> <span class="c-article-meta-recommendations__date">14 February 2020</span> </div> </div> </article> </div> </div> </section> <script> window.dataLayer = window.dataLayer || []; window.dataLayer.push({ recommendations: { recommender: 'semantic', model: 'specter', policy_id: 'NA', timestamp: 1732738854, embedded_user: 'null' } }); </script> <div class="main-content"> <section data-title="Main"><div class="c-article-section" id="Sec1-section"><h2 class="c-article-section__title js-section-title js-c-reading-companion-sections-item" id="Sec1">Main</h2><div class="c-article-section__content" id="Sec1-content"><p>During high-order harmonic generation (HHG) in gas<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 7" title="Lewenstein, M., Balcou, P., Ivanov, M. Y., L’Huillier, A. &amp; Corkum, P. B. Theory of high-harmonic generation by low-frequency laser fields. Phys. Rev. A 49, 2117–2132 (1994)." href="/articles/nphys281#ref-CR7" id="ref-link-section-d25713248e518">7</a></sup>, short electron wavepackets (EWPs) are periodically released by high-field ionization. Their subsequent coherent interaction with the remaining bound wavefunction leads to coherent extreme-ultraviolet (XUV) emission. The <i>T</i><sub>0</sub>/2 periodicity of this process (<i>T</i><sub>0</sub> being the laser optical period) ensures that only odd harmonics of the fundamental radiation are emitted. Temporally, the XUV pulses are emitted as a train of chirped attosecond pulses<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 8" title="Farkas, G. &amp; Tóth, C. Proposal for attosecond light pulse generation using laser induced multiple-harmonic conversion processes in rare gases. Phys. Lett. A 168, 447–450 (1992)." href="/articles/nphys281#ref-CR8" id="ref-link-section-d25713248e530">8</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 9" title="Paul, P. M. et al. Observation of a train of attosecond pulses from high harmonic generation. Science 292, 1689–1692 (2001)." href="/articles/nphys281#ref-CR9" id="ref-link-section-d25713248e533">9</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 10" title="Mairesse, Y. et al. Attosecond synchronization of high-harmonic soft x-rays. Science 302, 1540–1543 (2003)." href="/articles/nphys281#ref-CR10" id="ref-link-section-d25713248e536">10</a></sup> (1&nbsp;attosecond=10<sup>−18</sup>&nbsp;s). For both plateau (low energy) and cut-off (high energy) harmonics, specific focusing conditions ensure that only a single attosecond pulse is emitted every half&nbsp;cycle<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 11" title="Antoine, P., L’Huillier, A. &amp; Lewenstein, M. Attosecond pulse trains using high-order harmonics. Phys. Rev. Lett. 77, 1234–1237 (1996)." href="/articles/nphys281#ref-CR11" id="ref-link-section-d25713248e543">11</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 12" title="Gaarde, M. B. &amp; Schafer, K. J. Space-time considerations in the phase locking of high harmonics. Phys. Rev. Lett. 89, 213901 (2002)." href="/articles/nphys281#ref-CR12" id="ref-link-section-d25713248e546">12</a></sup>.</p><p>Extracting an isolated attosecond pulse from this train requires breaking the periodicity of the process, so that XUV emission is only possible within a single half cycle of the fundamental pulse. In this way, isolated 250-attosecond-long pulses were recently obtained<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 13" title="Kienberger, R. et al. Atomic transient recorder. Nature 427, 817–821 (2004)." href="/articles/nphys281#ref-CR13" id="ref-link-section-d25713248e553">13</a></sup> by selecting the (highly intensity dependent) cut-off harmonics generated in neon by a 5-fs linearly polarized, fundamental pulse with stabilized carrier-envelope phase (CEP). With this technique, the minimum pulse duration achievable is limited by the (<span class="stix">∼</span>10 eV) bandwidth of the selected cut-off harmonics, which prevents us reaching the sub-100-attosecond domain.</p><p>To isolate a broadband attosecond pulse, we used a different approach<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 2" title="Corkum, P. B., Burnett, N. H. &amp; Ivanov, M. Y. Subfemtosecond pulses. Opt. Lett. 19, 1870–1872 (1994)." href="/articles/nphys281#ref-CR2" id="ref-link-section-d25713248e560">2</a></sup>. Our approach relies on the strong HHG sensitivity on the ellipticity, <i>ɛ</i>, of the fundamental field, which is largely wavelength independent. The HHG efficiency is maximum when <i>ɛ</i>=0 (linear polarization) and decreases quickly as <i>ɛ</i> increases. Carrying out HHG with a fundamental pulse that is only linearly polarized for a short time (and elliptically polarized elsewhere) ensures that the XUV emission is temporally confined<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 2" title="Corkum, P. B., Burnett, N. H. &amp; Ivanov, M. Y. Subfemtosecond pulses. Opt. Lett. 19, 1870–1872 (1994)." href="/articles/nphys281#ref-CR2" id="ref-link-section-d25713248e573">2</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 14" title="Platonenko, V. T. &amp; Strelkov, V. Single attosecond soft-x-ray pulse generated with a limited laser beam. J. Opt. Soc. Am. B 16, 435–440 (1999)." href="/articles/nphys281#ref-CR14" id="ref-link-section-d25713248e576">14</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 15" title="Altucci, C. et al. Frequency-resolved time-gated high-order harmonics. Phys. Rev. A 58, 3934–3941 (1998)." href="/articles/nphys281#ref-CR15" id="ref-link-section-d25713248e579">15</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 16" title="Tcherbakoff, O. et al. Time gated high order harmonic generation. Phys. Rev. A 68, 043804 (2003)." href="/articles/nphys281#ref-CR16" id="ref-link-section-d25713248e582">16</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 17" title="Kovacev, M. et al. Temporal confinement of the harmonic emission through polarization gating. Eur. Phys. J. D 26, 79–82 (2003)." href="/articles/nphys281#ref-CR17" id="ref-link-section-d25713248e585">17</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 18" title="López-Martens, R. et al. Time-resolved ellipticity gating of high-order harmonic emission. Phys. Rev.&nbsp;A 69, 053811 (2004)." href="/articles/nphys281#ref-CR18" id="ref-link-section-d25713248e588">18</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 19" title="Chang, Z. Single attosecond pulse and xuv supercontinuum in the high-order harmonic plateau. Phys. Rev.&nbsp;A 70, 043802 (2004)." href="/articles/nphys281#ref-CR19" id="ref-link-section-d25713248e592">19</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 20" title="Strelkov, V. et al. Generation of attosecond pulses with ellipticity-modulated fundamental. Appl. Phys.&nbsp;B 78, 879–884 (2004)." href="/articles/nphys281#ref-CR20" id="ref-link-section-d25713248e595">20</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 21" title="Shan, B., Ghimire, S. &amp; Chang, Z. Generation of the attosecond extreme ultraviolet supercontinuum by a polarization gating. J. Mod. Opt. 52, 277–283 (2005)." href="/articles/nphys281#ref-CR21" id="ref-link-section-d25713248e598">21</a></sup> inside a ‘polarization gate’, where the fundamental ellipticity is&nbsp;small.</p><p>To modulate the laser-pulse polarization, we developed a simple technique<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 16" title="Tcherbakoff, O. et al. Time gated high order harmonic generation. Phys. Rev. A 68, 043804 (2003)." href="/articles/nphys281#ref-CR16" id="ref-link-section-d25713248e605">16</a></sup> using birefringent plates (see the <a data-track="click" data-track-label="link" data-track-action="section anchor" href="/articles/nphys281#Sec2">Methods</a> section). The polarization-gate width<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 22" title="Strelkov, V. et al. Single attosecond pulse production with an ellipticity-modulated driving IR pulse. J.&nbsp;Phys.&nbsp;B 38, L161–L167 (2005)." href="/articles/nphys281#ref-CR22" id="ref-link-section-d25713248e612">22</a></sup>, <i>τ</i><sub>g</sub>, given&nbsp;by </p><div id="Equ1" class="c-article-equation"><div class="c-article-equation__content"><img src="//media.springernature.com/lw372/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Equ1_HTML.gif" class="u-display-block" alt=""></div></div><p> (<i>ɛ</i><sub>thr</sub> being a threshold ellipticity, <i>τ</i> the minimum driving-pulse duration) can be controlled through a delay (<i>δ</i>) and an angle (<i>β</i>). For polarization gates as short as <i>T</i><sub>0</sub>/2, required to produce isolated attosecond pulses, the CEP<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 4" title="Baltuška, A. et al. Attosecond control of electronic process by intense light fields. Nature 421, 611–615 (2003)." href="/articles/nphys281#ref-CR4" id="ref-link-section-d25713248e647">4</a></sup> of the driving pulse also plays a crucial role in controlling the EWP dynamics<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 19" title="Chang, Z. Single attosecond pulse and xuv supercontinuum in the high-order harmonic plateau. Phys. Rev.&nbsp;A 70, 043802 (2004)." href="/articles/nphys281#ref-CR19" id="ref-link-section-d25713248e651">19</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 20" title="Strelkov, V. et al. Generation of attosecond pulses with ellipticity-modulated fundamental. Appl. Phys.&nbsp;B 78, 879–884 (2004)." href="/articles/nphys281#ref-CR20" id="ref-link-section-d25713248e654">20</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 22" title="Strelkov, V. et al. Single attosecond pulse production with an ellipticity-modulated driving IR pulse. J.&nbsp;Phys.&nbsp;B 38, L161–L167 (2005)." href="/articles/nphys281#ref-CR22" id="ref-link-section-d25713248e657">22</a></sup>. The CEP, controlling the field position in the envelope, locates the possible recombination times (linked to the field) inside or outside the gate (linked to the envelope). Here, we use our robust polarization modulator in conjunction with CEP-stabilized 5-fs pulses to create a polarization gate shorter than <i>T</i><sub>0</sub>/2. We observe the signature of the EWP dynamic control by recording the CEP dependence of the emitted XUV&nbsp;spectra.</p><p>Without polarization-induced confinement, we observed well-defined harmonics (we obtained 0.6-eV-wide plateau harmonics with both plates at <i>α</i>=<i>β</i>=45<sup><span class="stix">∘</span></sup>) that were weakly affected by the CEP, except for the cut-off harmonics generated in neon<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 23" title="Nisoli, M. et al. Effects of carrier-envelope phase differences of few-optical-cycle light pulses in single-shot high-order-harmonic spectra. Phys. Rev. Lett. 91, 213905 (2003)." href="/articles/nphys281#ref-CR23" id="ref-link-section-d25713248e677">23</a></sup>. When decreasing <i>β</i>, the interaction parameters were kept constant, except for the gate width, which was continuously decreased, and we observed a progressive broadening of the harmonics associated with a growing dependence on the CEP. With strong polarization-induced confinement, the CEP influence was very strong on the whole spectrum. <a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig1">Figure&nbsp;1</a> shows 50 XUV spectra (horizontal lines) generated in argon (with <i>τ</i>=5&nbsp;fs, <i>δ</i>=6.2&nbsp;fs, <i>β</i>=0<sup><span class="stix">∘</span></sup>) for 50 different CEP values varied over a 3π range. The spectra amplitudes and shapes periodically change for a CEP variation Δ<i>ψ</i>=π. For those CEP minimizing the XUV emission, clear harmonic structures are present. After a π/2 CEP shift, the efficiency becomes maximum, the harmonic structures vanish and the spectra become continuous in the range observed, with weak modulations for the lowest harmonics. For the cut-off part of the spectrum, the energy in the XUV continuum is estimated<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 24" title="Poletto, L., Bonora, S., Pascolini, M. &amp; Villoresi, P. Instrumentation for analysis and utilization of extreme-ultraviolet and soft x-ray high-order harmonics. Rev. Sci. Instrum. 75, 4413–4418 (2004)." href="/articles/nphys281#ref-CR24" id="ref-link-section-d25713248e703">24</a></sup> to be <span class="stix">∼</span>20 pJ per shot (efficiency:10<sup>−7</sup>) and for the 25–50 eV spectral range, the total XUV energy per shot is <span class="stix">∼</span>70 pJ.</p><div class="c-article-section__figure js-c-reading-companion-figures-item" data-test="figure" data-container-section="figure" id="figure-1" data-title="Spectra generated in argon."><figure><figcaption><b id="Fig1" class="c-article-section__figure-caption" data-test="figure-caption-text">Figure 1: Spectra generated in argon.</b></figcaption><div class="c-article-section__figure-content"><div class="c-article-section__figure-item"><a class="c-article-section__figure-link" data-test="img-link" data-track="click" data-track-label="image" data-track-action="view figure" href="/articles/nphys281/figures/1" rel="nofollow"><picture><source type="image/webp" srcset="//media.springernature.com/lw685/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Fig1_HTML.jpg?as=webp"><img aria-describedby="Fig1" src="//media.springernature.com/lw685/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Fig1_HTML.jpg" alt="figure 1" loading="lazy" width="369" height="301"></picture></a></div><div class="c-article-section__figure-description" data-test="bottom-caption" id="figure-1-desc"><p>Spectra emitted from an argon medium irradiated with a polarization-modulated pulse (<i>τ</i>=5&nbsp;fs, <i>δ</i>=6.2&nbsp;fs, <i>β</i>=0<sup><span class="stix">∘</span></sup>) as a function of the CEP shift. For some CEPs, harmonic peaks appear, whereas for other CEPs, they broaden up to a continuum.</p></div></div><div class="u-text-right u-hide-print"><a class="c-article__pill-button" data-test="article-link" data-track="click" data-track-label="button" data-track-action="view figure" href="/articles/nphys281/figures/1" data-track-dest="link:Figure1 Full size image" aria-label="Full size image figure 1" rel="nofollow"><span>Full size image</span><svg width="16" height="16" focusable="false" role="img" aria-hidden="true" class="u-icon"><use xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="#icon-eds-i-chevron-right-small"></use></svg></a></div></figure></div><p>When generating XUV in neon (using the same polarization modulation but a higher intensity in the gas medium), a stronger CEP influence was observed (<a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig2">Fig.&nbsp;2</a>). The emission efficiency still evolves with the same π periodicity but changes more strongly with the CEP. At maximum efficiency, the spectra were again continuous over all of the recorded bandwidths with a 30-eV full-width at half-maximum, and the energy in the continuum was <span class="stix">∼</span>1 pJ (efficiency: 5×10<sup>−9</sup>).</p><div class="c-article-section__figure js-c-reading-companion-figures-item" data-test="figure" data-container-section="figure" id="figure-2" data-title="Spectra generated in neon."><figure><figcaption><b id="Fig2" class="c-article-section__figure-caption" data-test="figure-caption-text">Figure 2: Spectra generated in neon.</b></figcaption><div class="c-article-section__figure-content"><div class="c-article-section__figure-item"><a class="c-article-section__figure-link" data-test="img-link" data-track="click" data-track-label="image" data-track-action="view figure" href="/articles/nphys281/figures/2" rel="nofollow"><picture><source type="image/webp" srcset="//media.springernature.com/lw685/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Fig2_HTML.jpg?as=webp"><img aria-describedby="Fig2" src="//media.springernature.com/lw685/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Fig2_HTML.jpg" alt="figure 2" loading="lazy" width="371" height="298"></picture></a></div><div class="c-article-section__figure-description" data-test="bottom-caption" id="figure-2-desc"><p>Spectra emitted from a neon medium irradiated with a polarization-modulated pulse (<i>τ</i>=5&nbsp;fs, <i>δ</i>=6.2&nbsp;fs, <i>β</i>=0<sup><span class="stix">∘</span></sup>) as a function of the CEP shift. The efficiency of the emission process strongly depends on the CEP, and the spectra are continuous at maximum efficiency.</p></div></div><div class="u-text-right u-hide-print"><a class="c-article__pill-button" data-test="article-link" data-track="click" data-track-label="button" data-track-action="view figure" href="/articles/nphys281/figures/2" data-track-dest="link:Figure2 Full size image" aria-label="Full size image figure 2" rel="nofollow"><span>Full size image</span><svg width="16" height="16" focusable="false" role="img" aria-hidden="true" class="u-icon"><use xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="#icon-eds-i-chevron-right-small"></use></svg></a></div></figure></div><p>Controlling <i>τ</i><sub>g</sub> by changing <i>δ</i> changed the XUV spectra dramatically. By reducing <i>δ</i> from 6.2 to 5&nbsp;fs (to increase <i>τ</i><sub>g</sub>) and generating XUV in neon, we observed an increase in the generation efficiency and a CEP evolution of the XUV spectra similar to that displayed in <a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig1">Fig.&nbsp;1</a> for argon with broad, but resolved, harmonics for some CEP values and broadband continuous spectra (reaching the 100 eV photon energy, and with an integrated energy of <span class="stix">∼</span>3 pJ per shot) for other CEP values. Slightly larger gates induced a large CEP-dependent harmonic frequency shift (also apparent in <a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig1">Fig.&nbsp;1</a> for the highest photon energy) that gives an apparent continuous spectrum without CEP stabilization. This clearly confirms that the observation of a continuous spectrum is only meaningful when the CEP is&nbsp;controlled<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 4" title="Baltuška, A. et al. Attosecond control of electronic process by intense light fields. Nature 421, 611–615 (2003)." href="/articles/nphys281#ref-CR4" id="ref-link-section-d25713248e803">4</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 19" title="Chang, Z. Single attosecond pulse and xuv supercontinuum in the high-order harmonic plateau. Phys. Rev.&nbsp;A 70, 043802 (2004)." href="/articles/nphys281#ref-CR19" id="ref-link-section-d25713248e806">19</a></sup>.</p><p>Decreasing <i>τ</i><sub>g</sub> by increasing <i>δ</i> allowed us to generate XUV continuous spectra, in argon, that show the strong modulation in efficiency formerly described with neon (<a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig2">Fig.&nbsp;2</a>). Increasing <i>δ</i> reduced the intensity in the gate, and thus decreased the emission&nbsp;efficiency.</p><p>We also verified the importance of selecting a single trajectory<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 11" title="Antoine, P., L’Huillier, A. &amp; Lewenstein, M. Attosecond pulse trains using high-order harmonics. Phys. Rev. Lett. 77, 1234–1237 (1996)." href="/articles/nphys281#ref-CR11" id="ref-link-section-d25713248e829">11</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 12" title="Gaarde, M. B. &amp; Schafer, K. J. Space-time considerations in the phase locking of high harmonics. Phys. Rev. Lett. 89, 213901 (2002)." href="/articles/nphys281#ref-CR12" id="ref-link-section-d25713248e832">12</a></sup> by properly positioning the medium after the laser focus, as the confinement effect was maximum there.</p><p>The strong CEP dependence of the spectra is consistent with a strong confinement of the XUV emission. For the highest harmonics generated in argon, either one or two XUV bursts, depending on the CEP, are emitted leading to either a continuous spectrum or a modulated spectrum with broad harmonic structures. The 1.6-eV width of the harmonics (<a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig3">Fig.&nbsp;3</a>b) is the signature of the interference between only two XUV bursts. For the lowest order harmonics obtained in argon (<a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig3">Fig.&nbsp;3</a>b), harmonic structures are always noticeable. This implies that these low harmonics are less confined (as expected from <a data-track="click" data-track-label="link" data-track-action="table anchor" href="/articles/nphys281#Tab1">Table&nbsp;1</a> because they are slightly less ellipticity sensitive) than the higher ones, and indicates that two pulses interfere. However, the observed modulation depth (10–20% of the signal) can be produced by a second attosecond pulse when its energy is less than 1% of the main-pulse energy. <a data-track="click" data-track-label="link" data-track-action="table anchor" href="/articles/nphys281#Tab1">Table&nbsp;1</a> shows that the high harmonics generated in neon are more ellipticity sensitive than those generated in argon. Therefore, the polarization-induced confinement is stronger for XUV emission in neon than in argon, as observed&nbsp;here.</p><div class="c-article-section__figure js-c-reading-companion-figures-item" data-test="figure" data-container-section="figure" id="figure-3" data-title="Comparison between simulated and experimental spectra."><figure><figcaption><b id="Fig3" class="c-article-section__figure-caption" data-test="figure-caption-text">Figure 3: Comparison between simulated and experimental spectra.</b></figcaption><div class="c-article-section__figure-content"><div class="c-article-section__figure-item"><a class="c-article-section__figure-link" data-test="img-link" data-track="click" data-track-label="image" data-track-action="view figure" href="/articles/nphys281/figures/3" rel="nofollow"><picture><source type="image/webp" srcset="//media.springernature.com/lw685/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Fig3_HTML.gif?as=webp"><img aria-describedby="Fig3" src="//media.springernature.com/lw685/springer-static/image/art%3A10.1038%2Fnphys281/MediaObjects/41567_2006_Article_BFnphys281_Fig3_HTML.gif" alt="figure 3" loading="lazy" width="400" height="330"></picture></a></div><div class="c-article-section__figure-description" data-test="bottom-caption" id="figure-3-desc"><p><b>a</b>, Simulated and <b>b</b>, experimental spectra obtained for HHG in argon with a polarization-modulated pulse (<i>τ</i>=5&nbsp;fs, <i>δ</i>=6.2&nbsp;fs, <i>β</i>=0<sup><span class="stix">∘</span></sup>) for two CEPs differing by π/2. The inset shows the simulated temporal profile associated with these CEPs (considering all of the harmonics above the order of 11 emitted in the laser direction from a 1-mm-thick argon jet).</p></div></div><div class="u-text-right u-hide-print"><a class="c-article__pill-button" data-test="article-link" data-track="click" data-track-label="button" data-track-action="view figure" href="/articles/nphys281/figures/3" data-track-dest="link:Figure3 Full size image" aria-label="Full size image figure 3" rel="nofollow"><span>Full size image</span><svg width="16" height="16" focusable="false" role="img" aria-hidden="true" class="u-icon"><use xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="#icon-eds-i-chevron-right-small"></use></svg></a></div></figure></div><div class="c-article-table" data-test="inline-table" data-container-section="table" id="table-1"><figure><figcaption class="c-article-table__figcaption"><b id="Tab1" data-test="table-caption">Table 1 Measured threshold ellipticity, <i>ɛ</i><sub>thr</sub>, for harmonic generation (order <b><i>q</i></b>=13&nbsp;to&nbsp;25) in argon and (<b><i>q</i></b>=27&nbsp;to&nbsp;73) in neon.</b></figcaption><div class="u-text-right u-hide-print"><a class="c-article__pill-button" data-test="table-link" data-track="click" data-track-action="view table" data-track-label="button" rel="nofollow" href="/articles/nphys281/tables/1" aria-label="Full size table 1"><span>Full size table</span><svg width="16" height="16" focusable="false" role="img" aria-hidden="true" class="u-icon"><use xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="#icon-eds-i-chevron-right-small"></use></svg></a></div></figure></div><p>The experimental results were simulated by a numerical model<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 14" title="Platonenko, V. T. &amp; Strelkov, V. Single attosecond soft-x-ray pulse generated with a limited laser beam. J. Opt. Soc. Am. B 16, 435–440 (1999)." href="/articles/nphys281#ref-CR14" id="ref-link-section-d25713248e1123">14</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 20" title="Strelkov, V. et al. Generation of attosecond pulses with ellipticity-modulated fundamental. Appl. Phys.&nbsp;B 78, 879–884 (2004)." href="/articles/nphys281#ref-CR20" id="ref-link-section-d25713248e1126">20</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 22" title="Strelkov, V. et al. Single attosecond pulse production with an ellipticity-modulated driving IR pulse. J.&nbsp;Phys.&nbsp;B 38, L161–L167 (2005)." href="/articles/nphys281#ref-CR22" id="ref-link-section-d25713248e1129">22</a></sup> derived from the three-steps model, including Coulomb attraction of the nucleus and propagation in the generating medium (1&nbsp;mm long). In <a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig3">Fig.&nbsp;3</a>a, we show two simulated spectra generated in argon (with <i>τ</i>=5&nbsp;fs, <i>δ</i>=6.2&nbsp;fs, <i>β</i>=0<sup><span class="stix">∘</span></sup>) for two CEP values differing by π/2. The corresponding experimental spectra are shown in <a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig3">Fig.&nbsp;3</a>b, and the overall agreement is striking. Only the fringe contrast is weaker experimentally than theoretically. This can be due to the fact that only on-axis emission is simulated (whereas the experimental spectra correspond to the XUV emission in all directions) and/or to the small (0.1 rad) CEP fluctuations. After selecting all of the harmonics with orders higher than 11 (experimentally this selection is possible with an Al filter), this analysis gives us the temporal shape of the XUV pulses (<a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig3">Fig.&nbsp;3</a>a inset). Changing the CEP leads to a situation where either two XUV attosecond pulses or a single attosecond burst (with a pre-pulse of energy equal to 0.5% of the main-pulse energy), which has a duration of 260 attoseconds (165 attoseconds after chirp compensation), are emitted. The simulations are also in good agreement with the results obtained in neon and show that, in the spectral range observed, chirped isolated pulses of 205 attoseconds (85 attoseconds after chirp compensation) can be produced over a broad range of CEP in the experimental conditions of <a data-track="click" data-track-label="link" data-track-action="figure anchor" href="/articles/nphys281#Fig2">Fig.&nbsp;2</a> (with very good contrast). Therefore, after chirp compensation, sub-100-attosecond XUV pulses are accessible with this technique. Chirp compensation was recently demonstrated<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 25" title="López-Martens, R. et al. Amplitude and phase control of attosecond light pulses. Phys. Rev. Lett. 94, 033001 (2005)." href="/articles/nphys281#ref-CR25" id="ref-link-section-d25713248e1157">25</a></sup> in the wavelength range corresponding to HHG in argon, and techniques have been published for other spectral&nbsp;domains<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 26" title="Kyung, T. K. et al. Single sub-50-attosecond pulse generation from chirp-compensated harmonic radiation using material dispersion. Phys. Rev. A 69, 051805 (2004)." href="/articles/nphys281#ref-CR26" id="ref-link-section-d25713248e1161">26</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 27" title="Chang, Z. Chirp of a single attosecond pulse generated by a polarization gating. Phys. Rev. A 71, 023813 (2005)." href="/articles/nphys281#ref-CR27" id="ref-link-section-d25713248e1164">27</a></sup>.</p><p>The generation of such broadband isolated EWP and XUV pulses opens the way for new applications in attoscience. Our approach enables us to vary the carrier wavelength of an isolated attosecond pulse, and therefore allows selective studies. For instance, at moderate XUV energy, isolated attosecond pulses can now be produced, and are well suited to follow ultrafast processes, such as proton transfer or evolution of highly excited molecular states. At higher energy, sub-100-attosecond pulses are within reach, and have the required duration to study electron–electron interactions, such as Auger processes or electron correlation. Trains of short EWPs were also directly used to carry out tomography of stationary molecular orbitals<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 5" title="Itatani, J. et al. Tomographic imaging of molecular orbitals. Nature 432, 867–871 (2004)." href="/articles/nphys281#ref-CR5" id="ref-link-section-d25713248e1171">5</a></sup>. Broadband, isolated short EWPs can be used to carry out time-resolved tomography of non-stationary molecular orbitals, or even to probe the ultrafast temporal evolution of bound&nbsp;EWPs<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 6" title="Nikura, H., Villeneuve, D. M. &amp; Corkum, P. B. Mapping attosecond electron wave packet motion. Phys. Rev. Lett. 94, 083003 (2005)." href="/articles/nphys281#ref-CR6" id="ref-link-section-d25713248e1175">6</a></sup>.</p><p>The energy of the isolated XUV pulses emitted through polarization gating can be increased in several ways. Here the generation parameters (gas pressure, interaction geometry, laser intensity) were chosen to unambiguously observe the confinement, and were probably not optimal for maximum efficiency. Higher-energy few-cycle pulses will also be available soon (through optical parametric chirped pulse amplification, OPCA, for instance) and can directly be used with this technique. Alternative polarization-gating techniques<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 2" title="Corkum, P. B., Burnett, N. H. &amp; Ivanov, M. Y. Subfemtosecond pulses. Opt. Lett. 19, 1870–1872 (1994)." href="/articles/nphys281#ref-CR2" id="ref-link-section-d25713248e1182">2</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 15" title="Altucci, C. et al. Frequency-resolved time-gated high-order harmonics. Phys. Rev. A 58, 3934–3941 (1998)." href="/articles/nphys281#ref-CR15" id="ref-link-section-d25713248e1185">15</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 28" title="Oron, D., Silberberg, Y., Dudovitch, N. &amp; Villeneuve, D. M. Efficient polarization gating of high-order harmonic generation by polarisation-shaped ultrashort pulses. Phys. Rev. A 72, 063816 (2006)." href="/articles/nphys281#ref-CR28" id="ref-link-section-d25713248e1188">28</a></sup> also exist, and could allow the use of longer fundamental pulses with higher energy. Finally, polarization gates shorter than <i>T</i><sub>0</sub>/2 are required here for the production of isolated attosecond pulses only because the periodicity of HHG is <i>T</i><sub>0</sub>/2. Adding a weak second-harmonic field to the fundamental pulse can increase this periodicity to <i>T</i><sub>0</sub>, in which case larger gates can be used which can be created with even higher-energy, longer fundamental&nbsp;pulses.</p><p>The XUV confinement to an isolated attosecond burst by polarization gating is possible both in the plateau and cut-off region because these harmonics evolve similarly with <i>ɛ</i>. This ellipticity dependence is very general, and we have shown that the central frequency of the attosecond pulse can be tuned by changing the gas. Other media can be used to further increase the bandwidth and tunability of isolated attosecond pulses. This bandwidth is limited by the cut-off energy, which has reached the keV level<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 29" title="Seres, J. et al. Source of coherent kiloelectronvolt X-rays. Nature 433, 596 (2005)." href="/articles/nphys281#ref-CR29" id="ref-link-section-d25713248e1210">29</a></sup> and can still be extended. Isolated pulses with a several-hundred-eV bandwidth, and a duration of a few attoseconds could then be obtained after chirp compensation, and will allow us to study ultrafast multiple-electron rearrangement. Using isolated broadband EWP, similar temporal resolution would be achievable for high-spatial-resolution tomography of electronic&nbsp;wavefunctions.</p></div></div></section><section data-title="Methods"><div class="c-article-section" id="Sec2-section"><h2 class="c-article-section__title js-section-title js-c-reading-companion-sections-item" id="Sec2">Methods</h2><div class="c-article-section__content" id="Sec2-content"><p>The polarization-gating technique that we have developed<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 16" title="Tcherbakoff, O. et al. Time gated high order harmonic generation. Phys. Rev. A 68, 043804 (2003)." href="/articles/nphys281#ref-CR16" id="ref-link-section-d25713248e1222">16</a></sup> provides both a rapid modulation of the ellipticity and a 100% transmission of the input pulse energy. It involves transmitting an incoming pulse through two birefringent (quartz) plates: a first thick plate and a zero-order quarter waveplate. The incoming pulse is linearly polarized (along a direction that defines the reference for the angles <i>α</i> and <i>β</i>) at <i>α</i>=45<sup><span class="stix">∘</span></sup> of the neutral axis of the first thick plate. By crossing it, the pulse is split into two delayed (delay <i>δ</i>) cross-polarized twin pulses. The delay, <i>δ</i>, is proportional to the plate thickness, and depends on the plate indexes at the carrier frequency of the pulse. Several thicknesses have been used to change <i>δ</i> (a 193-μm thickness induced <i>δ</i>=6.2&nbsp;fs at the carrier wavelength of 750&nbsp;nm). Alternatively, we also replaced this plate with two mobile quartz wedges (birefringent plate with controllable thickness) to continuously control <i>δ</i>. When necessary, we could tune the plate thickness to obtain a quarter waveplate at the pulse carrier wavelength. In that case, the outgoing pulse polarization evolves from linear to circular, and back to linear. After crossing a second zero-order broadband quarter waveplate (with its neutral axis at an angle <i>β</i> with respect to the reference direction), the outgoing pulse is linearly polarized at its centre and circularly polarized (for <i>β</i>=0<sup><span class="stix">∘</span></sup>) in its wings. Therefore, it has a time-dependent polarization, suitable for confining HHG. The polarization modulation is defined by <i>δ</i>, and by the minimum driving-pulse duration <i>τ</i> (we only consider pulses that are Fourier-limited in the interaction region). By considering gaussian pulses and defining the threshold ellipticity (see <a data-track="click" data-track-label="link" data-track-action="table anchor" href="/articles/nphys281#Tab1">Table&nbsp;1</a>), <i>ɛ</i><sub>thr</sub>, as the constant ellipticity for which the harmonic signal is decreased to 50% of the maximum signal (obtained for <i>ɛ</i>=0), the polarization gate has a width given by<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 22" title="Strelkov, V. et al. Single attosecond pulse production with an ellipticity-modulated driving IR pulse. J.&nbsp;Phys.&nbsp;B 38, L161–L167 (2005)." href="/articles/nphys281#ref-CR22" id="ref-link-section-d25713248e1279">22</a></sup> <i>τ</i><sub>g</sub>=<i>ɛ</i><sub>thr</sub><i>τ</i><sup>2</sup>/(ln(2)<i>δ</i>). Isolating a single attosecond pulse requires <i>τ</i><sub>g</sub>&lt;<i>T</i><sub>0</sub>/2. When the first quartz waveplate is a quarter waveplate, the gate width can be controlled further<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 16" title="Tcherbakoff, O. et al. Time gated high order harmonic generation. Phys. Rev. A 68, 043804 (2003)." href="/articles/nphys281#ref-CR16" id="ref-link-section-d25713248e1307">16</a></sup> by <i>β</i> without changing the intensity profile of the outgoing pulse. Larger gate widths, given by equation&nbsp;(1) can then be&nbsp;obtained.</p><p>As HHG is a highly nonlinear process, it is important to keep the highest intensity inside the gate to maximize the efficiency. Ideally, the peak intensity of the pulse must be reached in the gate, which implies <i>δ</i>≤<i>τ</i>. When delays larger than <i>τ</i> are used, the intensity shows a minimum inside the gate, and the polarization confinement can be influenced by a pre-pulse of higher intensity. Combining <i>δ</i>≤<i>τ</i> with <i>τ</i><sub>g</sub><span class="stix">∼</span><i>T</i><sub>0</sub>/2 requires pulses shorter than 6–7&nbsp;fs to efficiently generate isolated attosecond&nbsp;pulses.</p><p>The 5-fs pulses are produced by compression<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 30" title="Nisoli, M. et al. Generation of high energy 10&nbsp;fs pulses by a new pulse compression technique. Appl. Phys. Lett. 68, 2793–2795 (1996)." href="/articles/nphys281#ref-CR30" id="ref-link-section-d25713248e1344">30</a></sup> of 25-fs light pulses generated by a Ti:sapphire laser system (0.7-mJ energy, 1-kHz repetition rate). Such compression involves spectral broadening of the pulses inside an argon-filled tapered hollow fibre followed by recompression using ultrabroadband chirped mirrors. The CEP of the driving pulses is stabilized using an experimental setup similar to that described by Baltuška <i>et al.</i> <sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 4" title="Baltuška, A. et al. Attosecond control of electronic process by intense light fields. Nature 421, 611–615 (2003)." href="/articles/nphys281#ref-CR4" id="ref-link-section-d25713248e1351">4</a></sup>, and the residual CEP fluctuations are about 0.1&nbsp;rad (r.m.s.). The CEP can be finely adjusted, without changing the pulse duration. The pulse polarization was then modulated with the above-mentioned technique. The XUV light is produced by focusing the polarization-modulated pulses onto an argon- or neon-gas jet created by a 400-μm-wide nozzle. The jet was positioned after the laser focus to select the short quantum trajectory by means of phase matching<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 11" title="Antoine, P., L’Huillier, A. &amp; Lewenstein, M. Attosecond pulse trains using high-order harmonics. Phys. Rev. Lett. 77, 1234–1237 (1996)." href="/articles/nphys281#ref-CR11" id="ref-link-section-d25713248e1355">11</a>,<a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 12" title="Gaarde, M. B. &amp; Schafer, K. J. Space-time considerations in the phase locking of high harmonics. Phys. Rev. Lett. 89, 213901 (2002)." href="/articles/nphys281#ref-CR12" id="ref-link-section-d25713248e1358">12</a></sup>. After pre-compensating for the plate’s dispersion, we systematically checked that the pulses were unchirped in the interaction region. The radiation is collected and analysed by means of a high-throughput flat-field grazing-incidence spectrometer using an open solar-blind bidimensional&nbsp;detector<sup><a data-track="click" data-track-action="reference anchor" data-track-label="link" data-test="citation-ref" aria-label="Reference 24" title="Poletto, L., Bonora, S., Pascolini, M. &amp; Villoresi, P. Instrumentation for analysis and utilization of extreme-ultraviolet and soft x-ray high-order harmonics. Rev. Sci. Instrum. 75, 4413–4418 (2004)." href="/articles/nphys281#ref-CR24" id="ref-link-section-d25713248e1362">24</a></sup>.</p><p>The experimental conditions were optimized to suppress any spectral broadening that was not directly connected to the confinement induced by the combined action of CEP and polarization gating (we used a moderate gas pressure and a low enough intensity to avoid spectral changes related to ionization). 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J. Sola, E. Mével, L. Elouga &amp; E. Constant</p></li><li id="Aff2"><p class="c-article-author-affiliation__address">General Physics Institute of Russian Academy of Sciences, 38 Vavilova st., Moscow 119991, Russia</p><p class="c-article-author-affiliation__authors-list">V. Strelkov</p></li><li id="Aff3"><p class="c-article-author-affiliation__address">Department of Information Engineering, CNR-INFM, Laboratory of Ultraviolet and X-ray Optical Research, University of Padova, Via Gradenigo, 6, 35131 Padova, Italy</p><p class="c-article-author-affiliation__authors-list">L. Poletto &amp; P. Villoresi</p></li><li id="Aff4"><p class="c-article-author-affiliation__address">Department of Physics, CNR-INFM, National Laboratory for Ultrafast and Ultraintense Optical Science, Politecnico of Milan, Piazza L. da Vinci 32, 20133 Milano, Italy</p><p class="c-article-author-affiliation__authors-list">E. Benedetti, J.-P. Caumes, S. Stagira, C. Vozzi, G. Sansone &amp; M. Nisoli</p></li></ol><div class="u-js-hide u-hide-print" data-test="author-info"><span class="c-article__sub-heading">Authors</span><ol class="c-article-authors-search u-list-reset"><li id="auth-I__J_-Sola-Aff1"><span class="c-article-authors-search__title u-h3 js-search-name">I. J. 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Constant</a>.</p></div></div></section><section data-title="Ethics declarations"><div class="c-article-section" id="ethics-section"><h2 class="c-article-section__title js-section-title js-c-reading-companion-sections-item" id="ethics">Ethics declarations</h2><div class="c-article-section__content" id="ethics-content"> <h3 class="c-article__sub-heading">Competing interests</h3> <p>The authors declare no competing financial interests.</p> </div></div></section><section data-title="Rights and permissions"><div class="c-article-section" id="rightslink-section"><h2 class="c-article-section__title js-section-title js-c-reading-companion-sections-item" id="rightslink">Rights and permissions</h2><div class="c-article-section__content" id="rightslink-content"><p class="c-article-rights"><a data-track="click" data-track-action="view rights and permissions" data-track-label="link" 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