Emergent Relativistic Effects in Condensed Matter
From Fundamental Aspects to Electronic Functionality

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29.04.2025

Substrate Polarization Alters the Jahn-Teller Effect in a Single Molecule


M. Frankerl, L.L. Patera, F. Giselbrecht, T. Frederiksen, J. Repp, A. Donarini

Physical Review Letters 134, 176203 (2025)

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 that 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.

Substrate Polarization Alters the Jahn-Teller Effect in a Single Molecule | Phys. Rev. Lett.

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