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Ultrafast, Multidimensional attenuated total reflectance spectroscopy of adsorbates at metal surfaces


Kraack, Jan Philip; Lotti, Davide; Hamm, Peter (2014). Ultrafast, Multidimensional attenuated total reflectance spectroscopy of adsorbates at metal surfaces. Journal of Physical Chemistry Letters, 5(13):2325-2329.

Abstract

Ultrafast dynamics of molecules at solid-liquid interfaces are of outstanding importance in chemistry and physics due to their involvement in processes of heterogeneous catalysis. We present a new spectroscopic approach to resolve coherent, time-resolved, two-dimensional (2D) vibrational spectra as well as ultrafast vibrational relaxation dynamics of molecules adsorbed on metallic thin films in contact with liquids. The setup is based on the technique of Attenuated Total Reflectance (ATR) spectroscopy which is used at interfaces between materials that exhibit different refractive indices. As a sample molecule we consider carbon monoxide adsorbed in different binding configurations on different metals and resolve its femtosecond vibrational dynamics. It is presented that mid-infrared, multi-dimensional ATR spectroscopy allows for obtaining a surface-sensitive characterization of adsorbates’ vibrational relaxation, spectral diffusion dynamics and simple inhomogeneity on the femtosecond timescale.

Abstract

Ultrafast dynamics of molecules at solid-liquid interfaces are of outstanding importance in chemistry and physics due to their involvement in processes of heterogeneous catalysis. We present a new spectroscopic approach to resolve coherent, time-resolved, two-dimensional (2D) vibrational spectra as well as ultrafast vibrational relaxation dynamics of molecules adsorbed on metallic thin films in contact with liquids. The setup is based on the technique of Attenuated Total Reflectance (ATR) spectroscopy which is used at interfaces between materials that exhibit different refractive indices. As a sample molecule we consider carbon monoxide adsorbed in different binding configurations on different metals and resolve its femtosecond vibrational dynamics. It is presented that mid-infrared, multi-dimensional ATR spectroscopy allows for obtaining a surface-sensitive characterization of adsorbates’ vibrational relaxation, spectral diffusion dynamics and simple inhomogeneity on the femtosecond timescale.

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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:19 June 2014
Deposited On:09 Oct 2014 08:54
Last Modified:21 Nov 2017 17:28
Publisher:American Chemical Society
ISSN:1948-7185
Funders:Swiss National Foundation (grant CRSII2_136205/1) and by the University Research Priority Program (URPP) for solar light to chemical energy conversion (LightChEC)
Publisher DOI:https://doi.org/10.1021/jz500978z

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