Spectral broadening in lithium niobate in a self-diffraction geometry using ultrashort pulses

We report on broadband light generation in the impulsive regime in an un-doped lithium niobate (LiNbO3) crystal by two femtosecond laser pulses (36 fs) from a Ti-sapphire laser amplifier. We systematically investigate the role of incident intensity on spectral broadening. At relatively low incident intensity (0.7 TW cm(-2)), spectral broadening in the transmitted beam occurs due to the combined effect of self-phase modulation and cross-phase modulation. At higher incident intensity (10.2 TW cm(-2)), we observe generation of as many as 21 anti-Stokes orders due to coherent anti-Stokes Raman scattering in self-diffraction geometry. Moreover, we observe order-dependent spectral broadening of anti-Stokes lines that may be attributed to the competition with other nonlinear optical effects like cross-phase modulation.