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Spatially Resolved Vibronic Excitations of an Isolated Adsorbed Organometallic Complex via Multiple Tunneling Channels

Xiangzhi Meng1,*, Kai Uwe Clausen2, Marie-Laure Bocquet3, Alexander Weismann1, Niklas Ide1, Felix Tuczek2, and Richard Berndt1

  • *Contact author: meng@physik.uni-kiel.de
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Phys. Rev. Lett. 135, 136202 – Published 24 September, 2025

DOI: https://doi.org/10.1103/xxtf-98vs

Abstract

Vibronic excitations of molecules at nanoscale interfaces are important for molecular electronics and spintronics and have therefore attracted considerable attention. For single molecules in mechanically controlled break junctions or in a scanning tunneling microscope (STM), vibronic excitations are typically described by a double-barrier tunneling junction model. In this model, a homogeneous electric field is considered and the atomic structure of the metal contacts is neglected. Here, we report experimental STM data of a new nonplanar organometallic complex, [Mo(CO)3(Pyridine3S3)], on Ag(111). Spatially resolved maps of the vibronic excitations show several features related to the reordering of the occupied molecular orbitals due to the rapidly decaying potential of the tip apex. Such rearrangement leads to a significant shift in the vibronic levels as the tip position is changed. These observations, together with our modelling results, demonstrate that the molecular orbitals can be controlled by the field of the STM tip, whose atomic-scale variation deserves more attention in studies of nonplanar molecules.

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Phys. Rev. Lett. 135, 136202– Published 24 September, 2025
  • Received 12 March 2025
  • Revised 18 July 2025
  • Accepted 28 August 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

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