Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule
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arXiv
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| Natura: | Preprint |
| Pubblicazione: |
2024
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| author | Driver, Taran Guo, Zhaoheng Isele, Erik Grell, Gilbert Ruberti, Marco ONeal, Jordan T. Alexander, Oliver Beauvarlet, Sandra Cesar, David Duris, Joseph Garratt, Douglas Larsen, Kirk A. Li, Siqi Kolorenč, Přemysl McCracken, Gregory A. Tuthill, Daniel Wang, Zifan Berrah, Nora Bostedt, Christoph Borne, Kurtis Cheng, Xinxin DiMauro, Louis F. Doumy, Gilles Franz, Paris L. Kamalov, Andrei Li, Xiang Lin, Ming-Fu Obaid, Razib Picón, Antonio Robles, River R. Rolles, Daniel Rudenko, Artem Shaikh, Moniruzzaman Slaughter, Daniel S. Sudar, Nicholas S. Thierstein, Emily Ueda, Kiyoshi Wang, Enliang Wang, Anna L. Weber, Thorsten Wolf, Thomas J. A. Young, Linda Zhang, Zhen Averbukh, Vitali Gessner, Oliver Bucksbaum, Philip H. Kling, Matthias F. Palacios, Alicia Martín, Fernando Marangos, Jon P. Walter, Peter Marinelli, Agostino Cryan, James P. |
| author_facet | Driver, Taran Guo, Zhaoheng Isele, Erik Grell, Gilbert Ruberti, Marco ONeal, Jordan T. Alexander, Oliver Beauvarlet, Sandra Cesar, David Duris, Joseph Garratt, Douglas Larsen, Kirk A. Li, Siqi Kolorenč, Přemysl McCracken, Gregory A. Tuthill, Daniel Wang, Zifan Berrah, Nora Bostedt, Christoph Borne, Kurtis Cheng, Xinxin DiMauro, Louis F. Doumy, Gilles Franz, Paris L. Kamalov, Andrei Li, Xiang Lin, Ming-Fu Obaid, Razib Picón, Antonio Robles, River R. Rolles, Daniel Rudenko, Artem Shaikh, Moniruzzaman Slaughter, Daniel S. Sudar, Nicholas S. Thierstein, Emily Ueda, Kiyoshi Wang, Enliang Wang, Anna L. Weber, Thorsten Wolf, Thomas J. A. Young, Linda Zhang, Zhen Averbukh, Vitali Gessner, Oliver Bucksbaum, Philip H. Kling, Matthias F. Palacios, Alicia Martín, Fernando Marangos, Jon P. Walter, Peter Marinelli, Agostino Cryan, James P. |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2411_01700 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule Driver, Taran Guo, Zhaoheng Isele, Erik Grell, Gilbert Ruberti, Marco ONeal, Jordan T. Alexander, Oliver Beauvarlet, Sandra Cesar, David Duris, Joseph Garratt, Douglas Larsen, Kirk A. Li, Siqi Kolorenč, Přemysl McCracken, Gregory A. Tuthill, Daniel Wang, Zifan Berrah, Nora Bostedt, Christoph Borne, Kurtis Cheng, Xinxin DiMauro, Louis F. Doumy, Gilles Franz, Paris L. Kamalov, Andrei Li, Xiang Lin, Ming-Fu Obaid, Razib Picón, Antonio Robles, River R. Rolles, Daniel Rudenko, Artem Shaikh, Moniruzzaman Slaughter, Daniel S. Sudar, Nicholas S. Thierstein, Emily Ueda, Kiyoshi Wang, Enliang Wang, Anna L. Weber, Thorsten Wolf, Thomas J. A. Young, Linda Zhang, Zhen Averbukh, Vitali Gessner, Oliver Bucksbaum, Philip H. Kling, Matthias F. Palacios, Alicia Martín, Fernando Marangos, Jon P. Walter, Peter Marinelli, Agostino Cryan, James P. Chemical Physics 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. |
| title | Attosecond Coherent Electron Motion in a Photoionized Aromatic Molecule |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2411.01700 |