Tunable sideband laser from cascaded four-wave mixing in thin glass for ultra-broadband femtosecond stimulated Raman spectroscopy

We demonstrate the generation of broadband up-converted multicolor array (BUMA) in a thin BK7 glass slide using two noncollinear weak near-IR laser pulses with various crossing angles. The BUMA signal arises from cubic nonlinear χ⁽³⁾:χ⁽³⁾ processes via cascaded four-wave mixing of the two incident beams. Broad and continuous tunability of BUMA is simply achieved by varying the time delay between the two pulses. We implement one of the BUMA sidebands as the probe pulse for femtosecond stimulated Raman spectroscopy and collect a solvent mixture anti-Stokes Raman spectrum with an ultrabroad detection range of ca. 100–4000 cm⁻¹.