Exploring ultra-fast charge transfer and vibronic coupling with N 1s RIXS maps of an aromatic molecule coupled to a semiconductor

Research output: Contribution to journalArticle

Abstract

We present for the first time two-dimensional resonant inelastic x-ray scattering (RIXS) maps of multilayer and monolayer bi-isonicotinic acid adsorbed on the rutile TiO2(110) single crystal surface. This enables the elastic channel to be followed over the lowest unoccupied molecular orbitals resonantly excited at the N 1s absorption edge. The data also reveal ultra-fast intramolecular vibronic coupling, particularly during excitation into the lowest unoccupied molecular orbital-derived resonance. Both elastic scattering and the vibronic coupling loss features are expected to contain the channel in which the originally excited electron is directly involved in the core-hole decay process. This allows RIXS data for a molecule coupled to a wide bandgap semiconductor to be considered in the same way as the core-hole clock implementation of resonant photoemission spectroscopy (RPES). However, contrary to RPES measurements, we find no evidence for the depletion of the participator channel under the conditions of ultra-fast charge transfer from the molecule to the substrate densities of states, on the time scale of the core-hole lifetime. These results suggest that the radiative core-hole decay processes in RIXS are not significantly modified by charge transfer on the femtosecond time scale in this system.

Details

Authors
  • James N. O'Shea
  • Karsten Handrup
  • Robert H. Temperton
  • Andrew J. Gibson
  • Alessandro Nicolaou
  • Nicolas Jaouen
Organisations
External organisations
  • University of Nottingham
  • Synchrotron SOLEIL
Research areas and keywords

Subject classification (UKÄ) – MANDATORY

  • Physical Chemistry
  • Atom and Molecular Physics and Optics
Original languageEnglish
Article number134705
JournalJournal of Chemical Physics
Volume147
Issue number13
Publication statusPublished - 2017 Oct 7
Publication categoryResearch
Peer-reviewedYes