Stimulated Raman scattering spectroscopy and χ(3)-nonlinear lasing effects in single crystals of aragonite (orthorhombic CaCO3)

Abstract

The present work gives a brief review of the nonlinear χ(2)- and χ(3)-lasing properties of SRS-active natural crystals (minerals) known so far. This compilation complements new results of a detailed investigation of Raman induced χ(3)-effects in aragonite single crystals (orthorhombic CaCO3) under single- and dual-wavelength picosecond excitation in the UV, visible and near-IR spectral ranges. The studied effects at room and cryogenic temperatures comprise Stokes and anti-Stokes combs of almost two octaves bandwidth, THG, SFG, as well as cascaded and cross-cascaded χ(3) ↔ χ(3) interactions. All recorded lasing χ(3)-components were identified and attributed to three observed SRS-promoting vibration modes ωSRS1 ≈ 1087 cm-1, ωSRS2 ≈ 152 cm-1, and ωSRS3 ≈ 205 cm-1 (at room temperature) of aragonite. Stimulated Raman scattering (SRS) investigations of minerals so far enrich the arsenal of SRS-active crystals, which can be applied to solve fundamental and applied tasks of modern laser physics and nonlinear optics.