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Ultrafast multi-dimensional attenuated total reflectance spectroscopy of adsorbates at metal surfaces

Type of publication Peer-reviewed
Publikationsform Original article (peer-reviewed)
Publication date 2014
Author Kraack Jan Philip, Lotti Davide, Hamm Peter,
Project Homogeneous photocatalytic water splitting
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Original article (peer-reviewed)

Journal J. Phys. Chem. Lett.
Page(s) 2325 - 2329
Title of proceedings J. Phys. Chem. Lett.
DOI 10.1021/jz500978z


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, 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, multidimensional ATR spectroscopy allows for obtaining a surface-sensitive characterization of adsorbates’ vibrational relaxation, spectral diffusion dynamics, and sample inhomogeneity on the femtosecond time scale.