Microscopic origin of twist-dependent electron transfer rate in bilayer graphene
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arXiv
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| Autores principales: | , |
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| Formato: | Preprint |
| Publicado: |
2024
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| _version_ | 1866929575701774336 |
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| author | Escalante, Leonardo Coello Limmer, David T. |
| author_facet | Escalante, Leonardo Coello Limmer, David T. |
| contents | Using molecular simulation and continuum dielectric theory, we consider how electrochemical kinetics are modulated by twist angle in bilayer graphene electrodes. By establishing a connection between twist angle and the screening length of charge carriers within the electrode, we investigate how tunable metallicity modifies the statistics of the electron transfer energy gap. Constant potential molecular simulations show that the activation free energy for electron transfer increases with screening length, leading to a non-monotonic dependence on the twist angle. The twist angle alters the density of states, tuning the number of thermally-accessible channels for electron transfer and the reorganization energy by affecting the stability of the vertically excited state through attenuated image charge interactions. Understanding these effects allows us to express the Marcus rate of interfacial electron transfer as a function of twist angle, consistent with a growing body of experimental observations. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2405_00783 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Microscopic origin of twist-dependent electron transfer rate in bilayer graphene Escalante, Leonardo Coello Limmer, David T. Statistical Mechanics Mesoscale and Nanoscale Physics Chemical Physics Using molecular simulation and continuum dielectric theory, we consider how electrochemical kinetics are modulated by twist angle in bilayer graphene electrodes. By establishing a connection between twist angle and the screening length of charge carriers within the electrode, we investigate how tunable metallicity modifies the statistics of the electron transfer energy gap. Constant potential molecular simulations show that the activation free energy for electron transfer increases with screening length, leading to a non-monotonic dependence on the twist angle. The twist angle alters the density of states, tuning the number of thermally-accessible channels for electron transfer and the reorganization energy by affecting the stability of the vertically excited state through attenuated image charge interactions. Understanding these effects allows us to express the Marcus rate of interfacial electron transfer as a function of twist angle, consistent with a growing body of experimental observations. |
| title | Microscopic origin of twist-dependent electron transfer rate in bilayer graphene |
| topic | Statistical Mechanics Mesoscale and Nanoscale Physics Chemical Physics |
| url | https://arxiv.org/abs/2405.00783 |