Heidelberg 2015 – scientific programme

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MO: Fachverband Molekülphysik

MO 22: Femtosecond Spectroscopy 3

MO 22.5: Talk

Friday, March 27, 2015, 12:00–12:15, PH/HS1

Surface-Enhanced, 2D Attenuated Total Reflectance Infrared Spectroscopy At Solid-Liquid Interfaces — •Jan Philip Kraack, Davide Lotti, and Peter Hamm — Department of Chemistry, University of Zürich, Winterthurerstrasse 190, CH-8057

Femtosecond dynamics of molecules at solid-liquid and solid-gas interfaces have recently gained considerable attention in nonlinear spectroscopy. We present recent advances towards establishing a new experimental method which is capable for resolving coherent, ultrafast two-dimensional (2D) infrared (IR) spectra of molecules adsorbed on metallic thin films.(1) The method is based on measuring Attenuated Total Reflectance (ATR) signals at solid-liquid interfaces using metals for immobilization of the samples. We present details of the femtosecond 2D ATR IR technique together with benchmarking results from small molecules as well as organic monolayers.(2) The nonlinear signals are investigated in terms of surface-enhancement effects(3) and environmental interactions. It is demonstrated that 2D ATR IR spectroscopy allows a surface-sensitive characterization of vibrational lifetimes, dephasing, spectral diffusion and sample inhomogeneity on the femtosecond timescale.

(1) Kraack, J. P.; Lotti, D.; Hamm, P., JPC Lett. 2014, 18, 2325.

(2) Kraack, J. P.; Lotti, D.; Hamm, P., in preparation.

(3) Donaldson, P. M.; Hamm, P., Angew. Chemie 2013, 125, 662.