DOE OSTI · 3391124
Attosecond response of molecules to impulsive ionization
Abstract
When matter interacts with energetic radiation it can undergo sudden, or impulsive, ionization. This process can drive chemical change and occurs widely in space and planetary atmospheres, yet its comprehensive description challenges our current theoretical and computational capabilities as it requires advanced treatment of electron correlation and nonadiabatic dynamics beyond the Born–Oppenheimer approximation. Here, in this study, we measure the response of the para-aminophenol molecule to sudden ionization. Using attosecond X-ray absorption spectroscopy, we resolve the ultrafast dynamics of the ionized molecule with atomic precision. A subfemtosecond decay corresponds to states undergoing non-radiative decay, whereas few-femtosecond oscillatory signatures are associated with electronic wavepacket motion in stable cation states that later couple to nuclear motion. We compare our measurement with state-of-the-art computational modelling, qualitatively reproducing the observed response across multiple timescales. These results provide a benchmark for computational models of sudden ionization and ultrafast charge motion in matter.
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Driver, Taran [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); et al.] (ORCID:0000000237616883), Guo, Zhaoheng (ORCID:0000000338738804), Isele, Erik, Grell, Gilbert (ORCID:0000000161035846), Ruberti, Marco (ORCID:0000000304243643), O’Neal, Jordan T. (ORCID:0009000951199308), Alexander, Oliver (ORCID:0000000182217382), Beauvarlet, Sandra (ORCID:0009000407460664), Cesar, David (ORCID:0000000336691854), Duris, Joseph (ORCID:0000000299301166), Garratt, Douglas (ORCID:0000000286379984), Larsen, Kirk A., Li, Siqi (ORCID:0000000212626292), Kolorenč, Přemysl (ORCID:0000000207474546), McCracken, Gregory A., Tuthill, Daniel (ORCID:0000000281010635), Wang, Zifan, Berrah, Nora (ORCID:0000000332311164), Bostedt, Christoph (ORCID:0000000181698639), Borne, Kurtis, Cheng, Xinxin (ORCID:0000000175868240), DiMauro, Louis F., Doumy, Gilles (ORCID:0000000186724138), Franz, Paris L., Kamalov, Andrei, Li, Xiang (ORCID:0000000183384123), Lin, Ming-Fu (ORCID:0000000180862484), Obaid, Razib, Pícon, Antonio (ORCID:0000000261423440), Robles, River R. (ORCID:0000000271524675), Rolles, Daniel (ORCID:0000000239653477), Rudenko, Artem (ORCID:0000000291548463), Shaikh, Moniruzzaman (ORCID:0000000239689007), Slaughter, Daniel S. (ORCID:0000000246214552), Sudar, Nicholas S., Thierstein, Emily, Ueda, Kiyoshi, Wang, Enliang (ORCID:0000000257036501), Wang, Anna L. (ORCID:0000000175150626), Weber, Thorsten (ORCID:0000000337562704), Wolf, Thomas J. A. (ORCID:0000000206411279), Young, Linda (ORCID:000000022251039X), Zhang, Zhen, Averbukh, Vitali (ORCID:0000000179990075), Gessner, Oliver (ORCID:0000000347092822), Bucksbaum, Philip H. (ORCID:0000000312585571), Kling, Matthias F., Palacios, Alicia, Martín, Fernando (ORCID:000000027529925X), Marangos, Jon P. (ORCID:0000000171696955), Walter, Peter (ORCID:0000000188391154), Marinelli, Agostino (ORCID:0000000272484652), Cryan, James P. (ORCID:0000000277760919). 2026-07-20. Attosecond response of molecules to impulsive ionization. https://doi.org/10.1038/s41567-026-03360-x
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