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Ti : Sapphire-Based Picosecond Visible-Infrared Sum-Frequency Spectroscopy from 9003100 cm-1

Volume 58, Number 12 (Dec. 2004) Page 1377-1384

Hore, Dennis K.; King, Jennifer L.; Moore, Fred G.; Alavi, David S.; Hamamoto, Mathew Y.; Richmond, Geraldine L.

Visible-infrared sum-frequency spectroscopy is ideally suited to the study of surfaces and interfaces. This paper introduces new sum-frequency spectroscopy instrumentation that we have developed with two novel features: (1) stable and robust infrared generation in the 900-3100 cm-1 (11-3.2 μm) region using an amplified Ti : sapphire oscillator with a home-built OPG/OPA, and (2) continuous tuning over either 900-2700 cm-1 (11-3.7 μm) or 1800-3100 cm-1 (5.5-3.2 μm) in a single experiment. All practical details of baseline correction issues due to the picosecond pulses (including variation in infrared (IR) energy, spatial and temporal overlap, Fresnel co- efficients) are addressed while demonstrating signal throughout this region from an amorphous gold surface. A sum-frequency spectrum from an oriented polymer is shown as a complete example of the data treatment, which reveals the vibrational modes accessible in this wavelength region.