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Plasmonic Substrates Do Not Promote Vibrational Energy Transfer at Solid-Liquid Interfaces.

Jan Philip Kraack1, Laurent Sévery1, S David Tilley1

  • 1Department of Chemistry, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.

The Journal of Physical Chemistry Letters
|December 14, 2017
PubMed
Summary

Investigating vibrational energy transfer in rhenium carbonyl complexes reveals that plasmonic effects do not influence transfer rates. This allows for direct measurement of intermolecular distances on surfaces, irrespective of plasmonic properties.

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Area of Science:

  • Surface science
  • Spectroscopy
  • Physical chemistry

Background:

  • Intermolecular vibrational energy transfer is crucial for understanding surface dynamics.
  • Ultrafast 2D Attenuated Total Reflectance Infrared (2D ATR IR) spectroscopy probes these dynamics at interfaces.
  • Plasmonic enhancement effects can influence spectroscopic measurements.

Purpose of the Study:

  • To investigate intermolecular vibrational energy transfer in rhenium carbonyl complexes at solid-liquid interfaces.
  • To determine the impact of plasmonic surface enhancement on vibrational energy transfer rates.
  • To assess the utility of vibrational energy transfer as a probe for intermolecular distances.

Main Methods:

  • Utilized ultrafast 2D Attenuated Total Reflectance Infrared (2D ATR IR) spectroscopy.
  • Employed isotopically mixed monolayers of rhenium carbonyl complexes.
  • Investigated systems with both dielectric and plasmonic materials to compare surface enhancement effects.

Main Results:

  • Plasmonic effects were found to have no significant impact on vibrational energy transfer rates under moderate surface enhancement (up to ca. 30).
  • The observed behavior aligns with the established image-dipole model.
  • Vibrational energy transfer rates were confirmed as a reliable indicator of intermolecular distances.

Conclusions:

  • Vibrational energy transfer rates at solid-liquid interfaces are independent of plasmonic properties within the studied enhancement regime.
  • The image-dipole model adequately explains the lack of plasmonic influence.
  • Intermolecular distances on surfaces can be accurately determined using vibrational energy transfer measurements, independent of surface plasmonics.