Probing autoionization decay lifetimes of the $\mathbf{4d^{-1}6\boldsymbol{\ell}}$ core-excited states in xenon using attosecond noncollinear four-wave-mixing spectroscopy
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| Format: | Preprint |
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2025
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| _version_ | 1866912520966504448 |
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| author | Puskar, Nicolette G. Rupprecht, Patrick Dvořák, Jan Lin, Yen-Cheng Greene, Avery E. Lucchese, Robert R. McCurdy, C. William Leone, Stephen R. Neumark, Daniel M. |
| author_facet | Puskar, Nicolette G. Rupprecht, Patrick Dvořák, Jan Lin, Yen-Cheng Greene, Avery E. Lucchese, Robert R. McCurdy, C. William Leone, Stephen R. Neumark, Daniel M. |
| contents | The decay of core-excited states is a sensitive probe of autoionization dynamics and correlation effects in many-electron systems, occurring on the fastest timescales. Xenon, with its dense manifold of autoionizing resonances that can be coupled with near-infrared light, provides a platform to investigate these processes. In this work, the autoionization decay lifetimes of $4d^{-1}6\ell$ $(\ell = s, p, d, ...)$ core-excited states in xenon atoms are probed with extreme ultraviolet (XUV) attosecond noncollinear four-wave-mixing (FWM) spectroscopy. The $4d^{-1}_{\{5/2,\, 3/2\}}6p$ XUV-bright states (optically dipole allowed) exhibit decay lifetimes of $\sim$6 fs, which is consistent with spectator-type decay. In contrast, the $4d^{-1}_{\{5/2,\, 3/2\}}6s$ and $4d^{-1}_{\{5/2,\, 3/2\}}6d$ XUV-dark states (optically dipole forbidden) show longer decay lifetimes of $\sim$20 fs. Photoionization calculations confirm that all core-hole states with $4d$ character should decay via spectator channels in $\leq$ 6 fs, suggesting that the apparent longer dark state decay times arise from an alternative mechanism. A few-level simulation of the FWM process shows that the inclusion of a nearby, longer-lived dark state can mimic the experimental FWM signal, suggesting population cycling with a second electronic state with non-$4d$ character. Ab-initio calculations support the presence of such multi-electron excited states in the 60$-$70 eV range. These results demonstrate that FWM signals can encode coupled-state dynamics when probing complex systems, highlighting the importance of combining theoretical and experimental approaches to disentangle accurate core-level decay pathways and lifetimes. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2508_03128 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Probing autoionization decay lifetimes of the $\mathbf{4d^{-1}6\boldsymbol{\ell}}$ core-excited states in xenon using attosecond noncollinear four-wave-mixing spectroscopy Puskar, Nicolette G. Rupprecht, Patrick Dvořák, Jan Lin, Yen-Cheng Greene, Avery E. Lucchese, Robert R. McCurdy, C. William Leone, Stephen R. Neumark, Daniel M. Atomic Physics The decay of core-excited states is a sensitive probe of autoionization dynamics and correlation effects in many-electron systems, occurring on the fastest timescales. Xenon, with its dense manifold of autoionizing resonances that can be coupled with near-infrared light, provides a platform to investigate these processes. In this work, the autoionization decay lifetimes of $4d^{-1}6\ell$ $(\ell = s, p, d, ...)$ core-excited states in xenon atoms are probed with extreme ultraviolet (XUV) attosecond noncollinear four-wave-mixing (FWM) spectroscopy. The $4d^{-1}_{\{5/2,\, 3/2\}}6p$ XUV-bright states (optically dipole allowed) exhibit decay lifetimes of $\sim$6 fs, which is consistent with spectator-type decay. In contrast, the $4d^{-1}_{\{5/2,\, 3/2\}}6s$ and $4d^{-1}_{\{5/2,\, 3/2\}}6d$ XUV-dark states (optically dipole forbidden) show longer decay lifetimes of $\sim$20 fs. Photoionization calculations confirm that all core-hole states with $4d$ character should decay via spectator channels in $\leq$ 6 fs, suggesting that the apparent longer dark state decay times arise from an alternative mechanism. A few-level simulation of the FWM process shows that the inclusion of a nearby, longer-lived dark state can mimic the experimental FWM signal, suggesting population cycling with a second electronic state with non-$4d$ character. Ab-initio calculations support the presence of such multi-electron excited states in the 60$-$70 eV range. These results demonstrate that FWM signals can encode coupled-state dynamics when probing complex systems, highlighting the importance of combining theoretical and experimental approaches to disentangle accurate core-level decay pathways and lifetimes. |
| title | Probing autoionization decay lifetimes of the $\mathbf{4d^{-1}6\boldsymbol{\ell}}$ core-excited states in xenon using attosecond noncollinear four-wave-mixing spectroscopy |
| topic | Atomic Physics |
| url | https://arxiv.org/abs/2508.03128 |