Vibrational energy transfer (VET) between two isotopologues of [Re(dcb)(CO)3Br] immobilized on a TiO2 surface is studied with the help of 2D IR spectroscopy in dependence of surface coverage. To dilute the molecules on the surface, and thereby control the intermolecular distances, two different diluents have been used: a third isotopologue of the same molecule and 4-cyanobenzoic acid. As expected, the VET rate decreases with dilution. For a quantitative investigation of the distance dependence of the VET rate, we analyze the data based on an excitonic model. This model reveals the typical 1/r6-distance dependence for a dimer of a donor and acceptor, similar to the nuclear Overhauser effect in NMR spectroscopy or Förster resonant energy transfer in electronic spectroscopy. However, VET becomes a collective phenomenon on the surface, with the existence of a network of coupled molecules and its disappearance below a percolation threshold, dominating the concentration dependence of the VET rate.
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A closer look into the distance dependence of vibrational energy transfer on surfaces using 2D IR spectroscopy
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21 October 2020
Research Article|
October 20 2020
A closer look into the distance dependence of vibrational energy transfer on surfaces using 2D IR spectroscopy
Ricardo Fernández-Terán
;
Ricardo Fernández-Terán
Department of Chemistry, University of Zurich
, Winterthurerstrasse 190, Zurich, Switzerland
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Peter Hamm
Peter Hamm
a)
Department of Chemistry, University of Zurich
, Winterthurerstrasse 190, Zurich, Switzerland
a)Author to whom correspondence should be addressed: peter.hamm@chem.uzh.ch
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a)Author to whom correspondence should be addressed: peter.hamm@chem.uzh.ch
Note: This paper is part of the JCP Special Topic on Coherent Multidimensional Spectroscopy.
J. Chem. Phys. 153, 154706 (2020)
Article history
Received:
August 18 2020
Accepted:
September 28 2020
Citation
Ricardo Fernández-Terán, Peter Hamm; A closer look into the distance dependence of vibrational energy transfer on surfaces using 2D IR spectroscopy. J. Chem. Phys. 21 October 2020; 153 (15): 154706. https://doi.org/10.1063/5.0025787
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