Development of a two-color picosecond optical parametric oscillator, pumped by a Nd:YAG laser mode locked using a nonlinear mirror, for doubly-resonant sum frequency generation spectroscopy

peer reviewedWe step up a doubly-resonant sum frequency generation (DR-SFG) spectrometer based on the use of an all-solid-state flash-lamp-pumped Nd:YAG laser that synchronously pumps two parametric oscillators. Pulses as short as 12 ps FWHM are generated by mode locking a Nd:YAG oscillator using a frequency doubling nonlinear mirror combined with a two-photon absorber. The available pump power is shared between a LiNbO3/AgGaS2 optical parametric oscillator (OPO), tunable from 3800 to 1100cm-1 and a BBO OPO tunable from 410 to 2600 nm. Spectral resolution and pulse are 2 and 3 cm-1 in the infrared and visible spectral ranges, respectively. First DR-SFG spectra of self-assembled monolayers on Au are presented