Multiple charge transfer driven complex reaction dynamics: covalent bonding meets van der Waals interactions
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| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866909987281829888 |
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| author | Dong, Ruichao Hu, Xiaoqing McGinnis, Owen Dennis Wang, Xincheng Zhang, Yikang Chen, Ahai Pier, Andreas Tsertsvadze, Alexander Ma, Huanyu Feng, Jinze Weiherer, Jessica Sommerlad, Laura Schmidt, Madeleine Melzer, Niklas Kraft, Noah Jacob, Sina Marie Shen, Zhenjie Walsh, Noelle Wang, Jianguo Dörner, Reinhard Ueda, Kiyoshi Wu, Yong Trinter, Florian Jahnke, Till Jiang, Yuhai |
| author_facet | Dong, Ruichao Hu, Xiaoqing McGinnis, Owen Dennis Wang, Xincheng Zhang, Yikang Chen, Ahai Pier, Andreas Tsertsvadze, Alexander Ma, Huanyu Feng, Jinze Weiherer, Jessica Sommerlad, Laura Schmidt, Madeleine Melzer, Niklas Kraft, Noah Jacob, Sina Marie Shen, Zhenjie Walsh, Noelle Wang, Jianguo Dörner, Reinhard Ueda, Kiyoshi Wu, Yong Trinter, Florian Jahnke, Till Jiang, Yuhai |
| contents | Ultrafast charge transfer (CT) processes redistribute electronic charge within and between molecular units and play a central role in many physical, chemical, and biological phenomena. However, the microscopic pathways of multiple CT events, including the coupled structural evolution and energy redistribution, are challenging to disentangle experimentally in complex systems. To obtain controlled insight into such dynamics, well-defined properties are required. Here, we investigate the N2Ar dimer, which combines a covalent bond with a weak van der Waals interaction, using site-selective synchrotron photoionization and coincident detection of electrons and ions. Combined with ab initio calculations, this approach enables step-by-step tracking of ultrafast CT and fragmentation dynamics. We find that the dimer's structural evolution triggers a second CT event, opening complex reaction pathways in which electrons are transferred back and forth between Ar and N2, through two nonadiabatic transitions involving conical intersections. These results demonstrate that sequential multiple CT-induced transitions, even in a simple dimer, provide controlled insight into nonadiabatic reaction mechanisms relevant to complex systems. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2511_14201 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Multiple charge transfer driven complex reaction dynamics: covalent bonding meets van der Waals interactions Dong, Ruichao Hu, Xiaoqing McGinnis, Owen Dennis Wang, Xincheng Zhang, Yikang Chen, Ahai Pier, Andreas Tsertsvadze, Alexander Ma, Huanyu Feng, Jinze Weiherer, Jessica Sommerlad, Laura Schmidt, Madeleine Melzer, Niklas Kraft, Noah Jacob, Sina Marie Shen, Zhenjie Walsh, Noelle Wang, Jianguo Dörner, Reinhard Ueda, Kiyoshi Wu, Yong Trinter, Florian Jahnke, Till Jiang, Yuhai Chemical Physics Ultrafast charge transfer (CT) processes redistribute electronic charge within and between molecular units and play a central role in many physical, chemical, and biological phenomena. However, the microscopic pathways of multiple CT events, including the coupled structural evolution and energy redistribution, are challenging to disentangle experimentally in complex systems. To obtain controlled insight into such dynamics, well-defined properties are required. Here, we investigate the N2Ar dimer, which combines a covalent bond with a weak van der Waals interaction, using site-selective synchrotron photoionization and coincident detection of electrons and ions. Combined with ab initio calculations, this approach enables step-by-step tracking of ultrafast CT and fragmentation dynamics. We find that the dimer's structural evolution triggers a second CT event, opening complex reaction pathways in which electrons are transferred back and forth between Ar and N2, through two nonadiabatic transitions involving conical intersections. These results demonstrate that sequential multiple CT-induced transitions, even in a simple dimer, provide controlled insight into nonadiabatic reaction mechanisms relevant to complex systems. |
| title | Multiple charge transfer driven complex reaction dynamics: covalent bonding meets van der Waals interactions |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2511.14201 |