A versatile femtosecond stimulated Raman spectroscopy setup with tunable pulses in the visible to near infrared

We demonstrate a versatile and efficient setup to perform femtosecond stimulated Raman spectroscopy (FSRS). Technical innovations are implemented to achieve the wavelength tunability for both the picosecond narrowband Raman pump pulse and femtosecond broadband Raman probe pulse. Using a simplified one-grating scheme in a home-built second harmonic bandwidth compressor followed by a two-stage noncollinear optical parametric amplifier, we tune the Raman pump pulse from ca. 480 to 750 nm. To generate the suitable Raman probe pulse in tandem, we rely on our recently demonstrated broadband up-converted multicolor array technique that readily provides tunable broadband laser sidebands across the visible to near-infrared range. This unique setup has unparalleled flexibility for conducting FSRS. We measure the ground-state Raman spectra of a cyclohexane standard using tunable pump-probe pairs at various wavelengths across the visible region. The best spectral resolution is ∼12 cm−1. By tuning the pump wavelength closer to the electronic absorption band of a photoacid pyranine in water, we observe the pre-resonantly enhanced Raman signal. The stimulated Raman gain of the 1627 cm−1 mode is increased by over 15 times.