Attosecond X-ray Core-level Chronoscopy of Aromatic Molecules
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arXiv
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| Autores principales: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Formato: | Preprint |
| Publicado: |
2024
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| author | Ji, Jia-Bao Guo, Zhaoheng Driver, Taran Trevisan, Cynthia S. Cesar, David Cheng, Xinxin Duris, Joseph Franz, Paris L. Glownia, James Gong, Xiaochun Hammerland, Daniel Han, Meng Heck, Saijoscha Hoffmann, Matthias Kamalov, Andrei Larsen, Kirk A. Li, Xiang Lin, Ming-Fu Liu, Yuchen McCurdy, C. William Obaid, Razib ONeal, Jordan T. Rescigno, Thomas N. Robles, River R. Sudar, Nicholas Walter, Peter Wang, Anna L. Wang, Jun Wolf, Thomas J. A. Zhang, Zhen Ueda, Kiyoshi Lucchese, Robert R. Marinelli, Agostino Cryan, James P. Wörner, Hans Jakob |
| author_facet | Ji, Jia-Bao Guo, Zhaoheng Driver, Taran Trevisan, Cynthia S. Cesar, David Cheng, Xinxin Duris, Joseph Franz, Paris L. Glownia, James Gong, Xiaochun Hammerland, Daniel Han, Meng Heck, Saijoscha Hoffmann, Matthias Kamalov, Andrei Larsen, Kirk A. Li, Xiang Lin, Ming-Fu Liu, Yuchen McCurdy, C. William Obaid, Razib ONeal, Jordan T. Rescigno, Thomas N. Robles, River R. Sudar, Nicholas Walter, Peter Wang, Anna L. Wang, Jun Wolf, Thomas J. A. Zhang, Zhen Ueda, Kiyoshi Lucchese, Robert R. Marinelli, Agostino Cryan, James P. Wörner, Hans Jakob |
| contents | Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, spectral congestion and spatial delocalization of valence electron wave functions set fundamental limits to the complexity of systems that can be studied and the information that can be retrieved, respectively. Using attosecond X-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: the photoelectron spectra remain atom-like, the measurements become element specific and the observed scattering dynamics originate from a point-like source. We exploit these unique features to reveal the effects of electronegativity and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N-1s and C-1s core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wavefunction with increasing electronegativity of the atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2402_17685 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Attosecond X-ray Core-level Chronoscopy of Aromatic Molecules Ji, Jia-Bao Guo, Zhaoheng Driver, Taran Trevisan, Cynthia S. Cesar, David Cheng, Xinxin Duris, Joseph Franz, Paris L. Glownia, James Gong, Xiaochun Hammerland, Daniel Han, Meng Heck, Saijoscha Hoffmann, Matthias Kamalov, Andrei Larsen, Kirk A. Li, Xiang Lin, Ming-Fu Liu, Yuchen McCurdy, C. William Obaid, Razib ONeal, Jordan T. Rescigno, Thomas N. Robles, River R. Sudar, Nicholas Walter, Peter Wang, Anna L. Wang, Jun Wolf, Thomas J. A. Zhang, Zhen Ueda, Kiyoshi Lucchese, Robert R. Marinelli, Agostino Cryan, James P. Wörner, Hans Jakob Chemical Physics Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, spectral congestion and spatial delocalization of valence electron wave functions set fundamental limits to the complexity of systems that can be studied and the information that can be retrieved, respectively. Using attosecond X-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: the photoelectron spectra remain atom-like, the measurements become element specific and the observed scattering dynamics originate from a point-like source. We exploit these unique features to reveal the effects of electronegativity and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N-1s and C-1s core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wavefunction with increasing electronegativity of the atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter. |
| title | Attosecond X-ray Core-level Chronoscopy of Aromatic Molecules |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2402.17685 |