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Ultrafast Vibrational Dynamics of CO Ligands on RuTPP/Cu(110) under Photodesorption Conditions

1
Surface Science Research Centre and Department of Chemistry, University of Liverpool, Liverpool L69 3BX, UK
2
Surface and Interface Science Laboratory, RIKEN, Wako, Saitama 351-0198, Japan
*
Author to whom correspondence should be addressed.
Surfaces 2019, 2(1), 117-130; https://doi.org/10.3390/surfaces2010010
Received: 16 December 2018 / Revised: 21 January 2019 / Accepted: 3 February 2019 / Published: 7 February 2019
(This article belongs to the Special Issue Photon Driven Dynamics at Surfaces)
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Abstract

We have studied CO coordinated to ruthenium tetraphenylporphyrin (RuTPP)/Cu(110) and directly adsorbed to Cu(110), using femtosecond pump-sum frequency probe spectroscopy, to alter the degree of electron-vibration coupling between the metal substrate and CO. We observe the facile femtosecond laser-induced desorption of CO from RuTPP/Cu(110), but not from Cu(110). A change in the vibrational transients, in the first few picoseconds, from a red- to blue-shift of the C–O stretching vibration under photodesorption conditions, was also observed. This drastic change can be explained, if the cause of the C–O frequency redshift of Cu(110) is not the usually-assumed anharmonic coupling to low frequency vibrational modes, but a charge transfer from hot electrons to the CO 2π* state. This antibonding state shifts to higher energies on RuTPP, removing the C–O redshift and, instead, reveals a blueshift, predicted to arise from electron-mediated coupling between the coherently excited internal stretch and low frequency modes in the system. View Full-Text
Keywords: adsorbate dynamics; pump-probe spectroscopy adsorbate dynamics; pump-probe spectroscopy
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).
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Omiya, T.; Kim, Y.; Raval, R.; Arnolds, H. Ultrafast Vibrational Dynamics of CO Ligands on RuTPP/Cu(110) under Photodesorption Conditions. Surfaces 2019, 2, 117-130.

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