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Molecule-specific interactions of diatomic adsorbates at metal-liquid interfaces


Kraack, Jan Philip; Kaech, Andres; Hamm, Peter (2017). Molecule-specific interactions of diatomic adsorbates at metal-liquid interfaces. Structural Dynamics, 4(4):044009.

Abstract

Ultrafast vibrational dynamics of small molecules on platinum (Pt) layers in water are investigated using 2D attenuated total reflectance IR spectroscopy. Isotope combinations of carbon monoxide and cyanide are used to elucidate inter-adsorbate and substrate-adsorbate interactions. Despite observed cross-peaks in the CO spectra, we conclude that the molecules are not vibrationally coupled. Rather, strong substrate-adsorbate interactions evoke rapid (similar to 2 ps) vibrational relaxation from the adsorbate into the Pt layer, leading to thermal cross-peaks. In the case of CN, vibrational relaxation is significantly slower (similar to 10 ps) and dominated by adsorbate-solvent interactions, while the coupling to the substrate is negligible.

Abstract

Ultrafast vibrational dynamics of small molecules on platinum (Pt) layers in water are investigated using 2D attenuated total reflectance IR spectroscopy. Isotope combinations of carbon monoxide and cyanide are used to elucidate inter-adsorbate and substrate-adsorbate interactions. Despite observed cross-peaks in the CO spectra, we conclude that the molecules are not vibrationally coupled. Rather, strong substrate-adsorbate interactions evoke rapid (similar to 2 ps) vibrational relaxation from the adsorbate into the Pt layer, leading to thermal cross-peaks. In the case of CN, vibrational relaxation is significantly slower (similar to 10 ps) and dominated by adsorbate-solvent interactions, while the coupling to the substrate is negligible.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:July 2017
Deposited On:09 Mar 2018 13:04
Last Modified:18 Apr 2018 11:49
Publisher:American Institute of Physics
ISSN:2329-7778
Funders:Swiss National Science Foundation, URRP LightChEC of the University of Zurich
OA Status:Gold
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1063/1.4978894
Project Information:
  • : FunderSNSF
  • : Grant ID
  • : Project TitleSwiss National Science Foundation
  • : Funder
  • : Grant ID
  • : Project TitleURRP LightChEC of the University of Zurich

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