Strong signature of electron-vibration coupling in molecules on Ag(111) triggered by tip-gated discharging

Chao Li (), Christoph Kaspar, Ping Zhou, Jung-Ching Liu, Outhmane Chahib, Thilo Glatzel, Robert Häner, Ulrich Aschauer, Silvio Decurtins, Shi-Xia Liu (), Michael Thoss, Ernst Meyer () and Rémy Pawlak ()
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Chao Li: University of Basel
Christoph Kaspar: University of Freiburg
Ping Zhou: University of Bern
Jung-Ching Liu: University of Basel
Outhmane Chahib: University of Basel
Thilo Glatzel: University of Basel
Robert Häner: University of Bern
Ulrich Aschauer: University of Bern
Silvio Decurtins: University of Bern
Shi-Xia Liu: University of Bern
Michael Thoss: University of Freiburg
Ernst Meyer: University of Basel
Rémy Pawlak: University of Basel

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Electron-vibration coupling is of critical importance for the development of molecular electronics, spintronics, and quantum technologies, as it affects transport properties and spin dynamics. The control over charge-state transitions and subsequent molecular vibrations using scanning tunneling microscopy typically requires the use of a decoupling layer. Here we show the vibronic excitations of tetrabromotetraazapyrene (TBTAP) molecules directly adsorbed on Ag(111) into an orientational glassy phase. The electron-deficient TBTAP is singly-occupied by an electron donated from the substrate, resulting in a spin 1/2 state, which is confirmed by a Kondo resonance. The TBTAP•− discharge is controlled by tip-gating and leads to a series of peaks in scanning tunneling spectroscopy. These occurrences are explained by combining a double-barrier tunneling junction with a Franck-Condon model including molecular vibrational modes. This work demonstrates that suitable precursor design enables gate-dependent vibrational excitations of molecules on a metal, thereby providing a method to investigate electron-vibration coupling in molecular assemblies without a decoupling layer.

Date: 2023
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DOI: 10.1038/s41467-023-41601-2

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