Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites
The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
American Physical Society
2025-01-01
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| Series: | Physical Review X |
| Online Access: | http://doi.org/10.1103/PhysRevX.15.011008 |
| _version_ | 1826865948184805376 |
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| author | Jun Wang Taran Driver Paris L. Franz Přemysl Kolorenč Emily Thierstein River R. Robles Erik Isele Zhaoheng Guo David Cesar Oliver Alexander Sandra Beauvarlet Kurtis Borne Xinxin Cheng Louis F. DiMauro Joseph Duris James M. Glownia Martin Graßl Paul Hockett Matthias Hoffman Andrei Kamalov Kirk A. Larsen Siqi Li Xiang Li Ming-Fu Lin Razib Obaid Philipp Rosenberger Peter Walter Thomas J. A. Wolf Jon P. Marangos Matthias F. Kling Philip H. Bucksbaum Agostino Marinelli James P. Cryan |
| author_facet | Jun Wang Taran Driver Paris L. Franz Přemysl Kolorenč Emily Thierstein River R. Robles Erik Isele Zhaoheng Guo David Cesar Oliver Alexander Sandra Beauvarlet Kurtis Borne Xinxin Cheng Louis F. DiMauro Joseph Duris James M. Glownia Martin Graßl Paul Hockett Matthias Hoffman Andrei Kamalov Kirk A. Larsen Siqi Li Xiang Li Ming-Fu Lin Razib Obaid Philipp Rosenberger Peter Walter Thomas J. A. Wolf Jon P. Marangos Matthias F. Kling Philip H. Bucksbaum Agostino Marinelli James P. Cryan |
| author_sort | Jun Wang |
| collection | DOAJ |
| description | The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene ion following ionization of the K shell of the two nonequivalent carbon sites with a subfemtosecond x-ray pulse. Using the angular streaking technique to track the Auger-Meitner decay, we observe temporal modulations of the emission, indicating the electronic coherence of the core-excited ionic states, and extract a 6.5±0.8 fs average lifetime of the core-level vacancies. A quantum-mechanical model is employed to interpret the measurement, and we find the observed temporal modulations are independent of charge density oscillations. This work opens a new regime of coherent electronic motion, beyond charge migration, where electronic coherence manifests in the nonlocal quantum correlation between atomic sites while charge density oscillation is absent. Our results broaden the landscape of electronic coherence in molecular systems. |
| first_indexed | 2025-02-16T21:51:14Z |
| format | Article |
| id | doaj.art-f6d6f6c978ad4b1b94e018f744a18fe7 |
| institution | Directory Open Access Journal |
| issn | 2160-3308 |
| language | English |
| last_indexed | 2025-02-16T21:51:14Z |
| publishDate | 2025-01-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review X |
| spelling | doaj.art-f6d6f6c978ad4b1b94e018f744a18fe72025-01-16T15:06:44ZengAmerican Physical SocietyPhysical Review X2160-33082025-01-0115101100810.1103/PhysRevX.15.011008Probing Electronic Coherence between Core-Level Vacancies at Different Atomic SitesJun WangTaran DriverParis L. FranzPřemysl KolorenčEmily ThiersteinRiver R. RoblesErik IseleZhaoheng GuoDavid CesarOliver AlexanderSandra BeauvarletKurtis BorneXinxin ChengLouis F. DiMauroJoseph DurisJames M. GlowniaMartin GraßlPaul HockettMatthias HoffmanAndrei KamalovKirk A. LarsenSiqi LiXiang LiMing-Fu LinRazib ObaidPhilipp RosenbergerPeter WalterThomas J. A. WolfJon P. MarangosMatthias F. KlingPhilip H. BucksbaumAgostino MarinelliJames P. CryanThe detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene ion following ionization of the K shell of the two nonequivalent carbon sites with a subfemtosecond x-ray pulse. Using the angular streaking technique to track the Auger-Meitner decay, we observe temporal modulations of the emission, indicating the electronic coherence of the core-excited ionic states, and extract a 6.5±0.8 fs average lifetime of the core-level vacancies. A quantum-mechanical model is employed to interpret the measurement, and we find the observed temporal modulations are independent of charge density oscillations. This work opens a new regime of coherent electronic motion, beyond charge migration, where electronic coherence manifests in the nonlocal quantum correlation between atomic sites while charge density oscillation is absent. Our results broaden the landscape of electronic coherence in molecular systems.http://doi.org/10.1103/PhysRevX.15.011008 |
| spellingShingle | Jun Wang Taran Driver Paris L. Franz Přemysl Kolorenč Emily Thierstein River R. Robles Erik Isele Zhaoheng Guo David Cesar Oliver Alexander Sandra Beauvarlet Kurtis Borne Xinxin Cheng Louis F. DiMauro Joseph Duris James M. Glownia Martin Graßl Paul Hockett Matthias Hoffman Andrei Kamalov Kirk A. Larsen Siqi Li Xiang Li Ming-Fu Lin Razib Obaid Philipp Rosenberger Peter Walter Thomas J. A. Wolf Jon P. Marangos Matthias F. Kling Philip H. Bucksbaum Agostino Marinelli James P. Cryan Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites Physical Review X |
| title | Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites |
| title_full | Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites |
| title_fullStr | Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites |
| title_full_unstemmed | Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites |
| title_short | Probing Electronic Coherence between Core-Level Vacancies at Different Atomic Sites |
| title_sort | probing electronic coherence between core level vacancies at different atomic sites |
| url | http://doi.org/10.1103/PhysRevX.15.011008 |
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