Abstract

The use of infrared-FEL allows adsorbate vibrational spectroscopy by IR-visible sum-frequency generation (SFG) beyond the frequency range accessible by benchtop IR lasers. Therefore, we synchronized a frequency doubled mode-locked YAG laser (532 nm) with the CLIO-FEL, which is tuneable from 2 to 17.5 μm. The feasibility is demonstrated by recording SFG-vibrational spectra near 5-μm of the CO adsorbate at the electrochemical interface Pt/HClO 4 solution containing CH 3OH. These spectra indicate the coexistence of linearly and doubly-bounded species. This work is a preliminary step towards adsorbate SFG-vibrational spectroscopy at longer wavelengths.

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