Substrate stabilization of Jahn-Teller distortion in a single molecule
Fuente:
arXiv
Guardado en:
| Autores principales: | , , , , , |
|---|---|
| Formato: | Preprint |
| Publicado: |
2024
|
| Materias: | |
| Acceso en línea: | |
| Etiquetas: |
Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
|
| _version_ | 1866916724198080512 |
|---|---|
| author | Frankerl, Moritz Patera, Laerte L. Giselbrecht, Felix Frederiksen, Thomas Repp, Jascha Donarini, Andrea |
| author_facet | Frankerl, Moritz Patera, Laerte L. Giselbrecht, Felix Frederiksen, Thomas Repp, Jascha Donarini, Andrea |
| contents | Charge-state transitions of a single Cu-phthalocyanine molecule adsorbed on an insulating layer of NaCl on Cu(111) are probed by means of alternate charging scanning tunneling microscopy. Real-space imaging of the electronic transitions reveals the Jahn-Teller distortion occurring upon formation of the first and second anionic charge states. The experimental findings are rationalized by a theoretical many-body model which highlights the crucial role played by the substrate. The latter enhances and stabilizes the intrinsic Jahn-Teller distortion of the negatively charged molecule hosting a degenerate pair of single-particle frontier orbitals. Consequently, two excess electrons are found to occupy, in the ground state, the same localized orbital, despite a larger Coulomb repulsion than the one for the competing delocalized electronic configuration. Control over the charging sequence by varying the applied bias voltage is also predicted. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2408_00478 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Substrate stabilization of Jahn-Teller distortion in a single molecule Frankerl, Moritz Patera, Laerte L. Giselbrecht, Felix Frederiksen, Thomas Repp, Jascha Donarini, Andrea Materials Science Mesoscale and Nanoscale Physics Charge-state transitions of a single Cu-phthalocyanine molecule adsorbed on an insulating layer of NaCl on Cu(111) are probed by means of alternate charging scanning tunneling microscopy. Real-space imaging of the electronic transitions reveals the Jahn-Teller distortion occurring upon formation of the first and second anionic charge states. The experimental findings are rationalized by a theoretical many-body model which highlights the crucial role played by the substrate. The latter enhances and stabilizes the intrinsic Jahn-Teller distortion of the negatively charged molecule hosting a degenerate pair of single-particle frontier orbitals. Consequently, two excess electrons are found to occupy, in the ground state, the same localized orbital, despite a larger Coulomb repulsion than the one for the competing delocalized electronic configuration. Control over the charging sequence by varying the applied bias voltage is also predicted. |
| title | Substrate stabilization of Jahn-Teller distortion in a single molecule |
| topic | Materials Science Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2408.00478 |