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.

中文翻译：

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文石（正交碳酸钙）单晶中的受激拉曼散射光谱和 χ(3)-非线性激光效应

目前的工作简要回顾了迄今为止已知的 SRS 活性天然晶体（矿物）的非线性 χ(2) 和 χ(3) 激光特性。该汇编补充了在紫外、可见光和近红外光谱范围内单波长和双波长皮秒激发下文石单晶（正交碳酸钙）中拉曼诱导 χ(3) 效应的详细研究的新结果。研究的室温和低温效应包括几乎两个倍频程带宽、THG、SFG 的斯托克斯和反斯托克斯梳，以及级联和交叉级联 χ(3) ↔ χ(3) 相互作用。所有记录的激光 χ(3) 分量都被识别并归因于文石的三种观察到的 SRS 促进振动模式 ωSRS1 ≈ 1087 cm-1、ωSRS2 ≈ 152 cm-1 和 ωSRS3 ≈ 205 cm-1（室温下）。