Ultrafast Relaxation Dynamics of Inner-Shell Vacancies in Hydrated Pyrrole
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arXiv
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| Main Authors: | , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866911240258846720 |
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| author | Wang, Kedong Wan, Bohui Covington, Cody L. Varga, Kalman |
| author_facet | Wang, Kedong Wan, Bohui Covington, Cody L. Varga, Kalman |
| contents | We employ real-space, real-time time-dependent density functional theory (TDDFT) combined with Ehrenfest dynamics to investigate ultrafast intermolecular relaxation following inner-valence ionization in hydrated pyrrole. This time-dependent approach treats electronic and nuclear motions simultaneously, allowing the description of electronic excitation, charge transfer, ionization, and nuclear motion.When the initial vacancy in the O 2s 1 state is created on the water molecule, the system predominantly undergoes intermolecular Coulombic decay (ICD) and electron-transfer mediated decay (ETMD), accompanied by pronounced charge transfer between pyrrole and water. In contrast, ionization of the pyrrole site for N 2s electron leads to both ICD and Auger decay channels. These results demonstrate that the decay dynamics are strongly governed by the initial vacancy location, offering microscopic insight into intermolecular energy-transfer mechanisms in hydrated molecular systems. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2510_25865 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Ultrafast Relaxation Dynamics of Inner-Shell Vacancies in Hydrated Pyrrole Wang, Kedong Wan, Bohui Covington, Cody L. Varga, Kalman Chemical Physics We employ real-space, real-time time-dependent density functional theory (TDDFT) combined with Ehrenfest dynamics to investigate ultrafast intermolecular relaxation following inner-valence ionization in hydrated pyrrole. This time-dependent approach treats electronic and nuclear motions simultaneously, allowing the description of electronic excitation, charge transfer, ionization, and nuclear motion.When the initial vacancy in the O 2s 1 state is created on the water molecule, the system predominantly undergoes intermolecular Coulombic decay (ICD) and electron-transfer mediated decay (ETMD), accompanied by pronounced charge transfer between pyrrole and water. In contrast, ionization of the pyrrole site for N 2s electron leads to both ICD and Auger decay channels. These results demonstrate that the decay dynamics are strongly governed by the initial vacancy location, offering microscopic insight into intermolecular energy-transfer mechanisms in hydrated molecular systems. |
| title | Ultrafast Relaxation Dynamics of Inner-Shell Vacancies in Hydrated Pyrrole |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2510.25865 |