Substrate stabilization of Jahn-Teller distortion in a single molecule
Abstract
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.
Cite
@article{arxiv.2408.00478,
title = {Substrate stabilization of Jahn-Teller distortion in a single molecule},
author = {Moritz Frankerl and Laerte L. Patera and Felix Giselbrecht and Thomas Frederiksen and Jascha Repp and Andrea Donarini},
journal= {arXiv preprint arXiv:2408.00478},
year = {2025}
}