Regensburg 2016 – scientific programme

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O: Fachverband Oberflächenphysik

O 33: Photonics and Nanooptics I: Infrared Spectroscopy

O 33.7: Talk

Tuesday, March 8, 2016, 12:00–12:15, H4

Ultrafast Vibrational Ladder Climbing on a Surface with 2D ATR IR Spectroscopy — •Jan Philip Kraack and Peter Hamm — Department of Chemistry, University of Zürich, Winterthurerstrasse 190, CH-8057

Vibrational dynamics of molecules at solid-liquid and solid-gas interfaces are important for various technical and scientific applications. In order to directly obtain multi-dimensional infrared (IR) spectra of adorbats at surfaces we have recently developed 2D Attenuated Total Reflection (ATR) IR spectroscopy.(1,2) Surface-enhancement effects in 2D ATR IR spectroscopy, stemming from plasmonic nano-structured noble-metal surfaces, have recently been characterized.(3) Here, we demonstrate optimized surface-enhancement for organic molecules on ultrathin (nm) metal surfaces which allows for vibrational ladder climbing (LC) in the electronic ground state potential of IR labels with even low extinction coefficients (< 200 M-1 cm-1). LC in such samples enables the characterization of ultrafast vibrational relaxation within the electronic ground state potential of a broad range of chemical bonds and is likely to be exploitable in coherent control(4) of surface-reactions.

(1) J.P. Kraack, D. Lotti and P. Hamm, J. Phys. Chem. Lett., 2014, 5, 2325-2329.

(2) J.P. Kraack, D. Lotti and P. Hamm, J. Chem. Phys., 2015, 142, 212413.

(3) J.P. Kraack and P. Hamm, submitted, 2015.

(4) T. Witte et al., J. Chem. Phys., 2003, 118, 2021-2024.