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

O'Shea, James N.; Handrup, Karsten; Temperton, Robert H.; Gibson, Andrew J.; Nicolaou, Alessandro; Jaouen, Nicolas

Authors

James N. O'Shea

Karsten Handrup

Robert H. Temperton

Andrew J. Gibson

Alessandro Nicolaou

Nicolas Jaouen



Abstract

We present for the first time two-dimensional resonant inelastic x-ray scattering (RIXS) maps of multilayer and monolayer biisonicotinic 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 reveals ultra-fast intramolecular vibronic coupling, particularly during excitation into the LUMO-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 depletion of the participator channel under the conditions of ultra-fast charge transfer from the molecule to the substrate densities of states, on the timescale 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 timescale in this system.

Journal Article Type Article
Journal Journal of Chemical Physics
Print ISSN 0021-9606
Electronic ISSN 1089-7690
Publisher AIP Publishing
Peer Reviewed Peer Reviewed
Volume 147
Issue 13
Article Number 134705
APA6 Citation O'Shea, J. N., Handrup, K., Temperton, R. H., Gibson, A. J., Nicolaou, A., & Jaouen, N. (in press). Exploring ultra-fast charge transfer and vibronic coupling with N 1s RIXS maps of an aromatic molecule coupled to a semiconductor. Journal of Chemical Physics, 147(13), https://doi.org/10.1063/1.4999135
DOI https://doi.org/10.1063/1.4999135
Publisher URL http://dx.doi.org/10.1063/1.4999135
Copyright Statement Copyright information regarding this work can be found at the following address: http://eprints.nottingh.../end_user_agreement.pdf
Additional Information This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. The following article appeared in The Journal of Chemical Physics 147, 134705 (2017); doi: 10.1063/1.4999135 and may be found at http://dx.doi.org/10.1063/1.4999135

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Copyright Statement
Copyright information regarding this work can be found at the following address: http://eprints.nottingham.ac.uk/end_user_agreement.pdf





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