Vibrationally resolved sum-frequency generation with broad-bandwidth infrared pulses

Abstract

We present a novel procedure for vibrationally resolved sum-frequency generation (SFG) in which a broad-bandwidth IR pulse is mixed with a narrow-bandwidth visible pulse. The resultant SFG spectrum is dispersed with a spectrograph and detected in parallel with a scientific-grade CCD detector, permitting rapid and high signal-to-noise ratio data acquisition over a 400-cm(-1) spectral region without scanning the IR frequency. Application to the study of a self-assembled monolayer of octadecanethiol is discussed.