Stimulated Raman scattering spectroscopy and χ~((3))-nonlinear lasing effects in single crystals of aragonite (orthorhombic CaCO_3)

摘要

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 CaCO_3) 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.