Manifestations of nonlinear optical effects in a novel SRS-active crystal—natural topaz, Al2(F1−x(OH)x)2SiO4: many-phonon χ(3)-lasing, more than sesqui-octave Stokes and anti-Stokes multi-wavelength comb lasing, cascaded and cross-cascaded χ(3)↔χ(3) Raman-induced interactions under single- and dual-wavelength picosecond collinear coherent pumping, THG and combined SRS-promoting phonon modes**On the 50th anniversary of the discovery of stimulated Raman scattering.

Abstract

Natural crystals of topaz, Al2(F1−x(OH)x)2SiO4 were found to be an attractive Raman gain material and a subject for the investigation of different χ(3)-nonlinear optical effects. We present several manifestations of photon–phonon interactions related to SRS and RFWM processes initiated by picosecond excitations at room and cryogenic (≈9 K) temperature. Among them are octave-spanning Stokes and anti-Stokes generation in the visible and near-IR spectral range, combined SRS-active phonon modes, cross-cascaded up-conversion, χ(3)↔χ(3) lasing, as well as THG via self-sum frequency parametric generation. All recorded Raman-induced lasing lines are identified and attributed to the promoting χ(3)-vibration transitions. Based on the experimental data, theoretical simulations employing Fourier analysis are performed to demonstrate the potential of wide SRS frequency combs in terms of ultra-short pulse generation.