Real-Time Coupled Electron-Nuclear Dynamics of Chemical Bond Formation: Hydrogen Scattering from a Semiconductor Surface
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| Main Authors: | , , , , , , |
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| Format: | Preprint |
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2025
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| _version_ | 1866915653012684800 |
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| author | Shi, Jialong Zhu, Lingjun Nitz, Florian Bünermann, Oliver Wodtke, Alec M. Guo, Hua Jiang, Bin |
| author_facet | Shi, Jialong Zhu, Lingjun Nitz, Florian Bünermann, Oliver Wodtke, Alec M. Guo, Hua Jiang, Bin |
| contents | A first-principles coupled electron-nuclear dynamics simulation based on real-time, time-dependent density functional theory and Ehrenfest dynamics quantitatively repro-duces bimodal translational energy loss and angular distributions observed in experiment for hydrogen atom scattering from Ge(111)-c(2*8). The theory elucidates a site-selective mechanism of electronically nonadiabatic energy transfer associated with the formation of different Ge-H bonds. When a hydrogen atom approaches a Ge rest-atom, it is strongly accelerated toward the potential minimum forming a transient Ge-H bond and then re-flected by the repulsive wall. This transient bond formation triggers an ultrafast electron transfer event from the rest-atom to an adjacent Ge-adatom, involving several crossings between valence and conduction bands of the substrate. Electronic equilibration is impos-sible within such a short time (Born-Oppenheimer failure) allowing the H-atom kinetic energy to be converted to inter-band electronic excitation of the substrate. H-atom colli-sions at other Ge atoms also form a transient bond but exhibit no electronic excitation, resulting in distinctly less efficient energy loss in scattered H-atoms. The nucle-ar-to-electronic energy transfer observed in this system reflects the electronic dynamics of covalent bond formation at a semiconductor surface, a mechanism that is quite distinct from previously identified nonadiabatic energy transfer mechanisms at metal surfaces mediated by electronic friction or transient negative ions. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2512_03753 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Real-Time Coupled Electron-Nuclear Dynamics of Chemical Bond Formation: Hydrogen Scattering from a Semiconductor Surface Shi, Jialong Zhu, Lingjun Nitz, Florian Bünermann, Oliver Wodtke, Alec M. Guo, Hua Jiang, Bin Chemical Physics Materials Science A first-principles coupled electron-nuclear dynamics simulation based on real-time, time-dependent density functional theory and Ehrenfest dynamics quantitatively repro-duces bimodal translational energy loss and angular distributions observed in experiment for hydrogen atom scattering from Ge(111)-c(2*8). The theory elucidates a site-selective mechanism of electronically nonadiabatic energy transfer associated with the formation of different Ge-H bonds. When a hydrogen atom approaches a Ge rest-atom, it is strongly accelerated toward the potential minimum forming a transient Ge-H bond and then re-flected by the repulsive wall. This transient bond formation triggers an ultrafast electron transfer event from the rest-atom to an adjacent Ge-adatom, involving several crossings between valence and conduction bands of the substrate. Electronic equilibration is impos-sible within such a short time (Born-Oppenheimer failure) allowing the H-atom kinetic energy to be converted to inter-band electronic excitation of the substrate. H-atom colli-sions at other Ge atoms also form a transient bond but exhibit no electronic excitation, resulting in distinctly less efficient energy loss in scattered H-atoms. The nucle-ar-to-electronic energy transfer observed in this system reflects the electronic dynamics of covalent bond formation at a semiconductor surface, a mechanism that is quite distinct from previously identified nonadiabatic energy transfer mechanisms at metal surfaces mediated by electronic friction or transient negative ions. |
| title | Real-Time Coupled Electron-Nuclear Dynamics of Chemical Bond Formation: Hydrogen Scattering from a Semiconductor Surface |
| topic | Chemical Physics Materials Science |
| url | https://arxiv.org/abs/2512.03753 |