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 ωSRS 1 ≈ 1087 cm–1, ωSRS 2 ≈ 152 cm–1, and ωSRS 3 ≈ 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. (© 2012 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA) (© 2011 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA)

Cerussite, PbCO3 – a new Stimulated Raman Scattering (SRS)‐active crystal with high‐order Stokes and anti‐Stokes lasing

“…For the excitation of single pass (cavity‐free) Raman‐induced Stokes and anti‐Stokes χ (3) ‐lasing of cerussite single crystals in the visible, near‐ and mid‐IR range, we used a SRS‐setup based on a home‐made Xe‐flashlamp pumped picosecond Nd 3+ :Y 3 Al 5 O 12 laser. Details of the setup and the methods of measurements are described in several recent publications (see, e.g., ). The used pump laser can emit at two fundamental wavelengths, λ f1 = 1.06415μm with pulse duration τ f1 ≈ 80 ps, or λ f2 = 0.53207 μm with τ f2 ≈ 60 ps.…”

“…The present work is devoted to the investigation of χ (3) ‐nonlinear laser SRS properties of another natural crystal, cerussite, PbCO 3 . The close structural similarity of cerussite to aragonite (CaCO 3 ), a crystal which offers several attractive manifestations of nonlinear laser interactions , motivated our SRS investigation of PbCO 3 .…”

Phosgenite, Pb2CO3Cl2 – a novel SRS‐active crystal

“…A common structural feature of the carbonates specified above is a coplanar, sheet-like arrangement of the isolated triangular [CO 3 ] groups, which alternate with sheets of M II cations in the crystal structures. The vibration modes of the [CO 3 ] groups, particularly the totally symmetric breathing mode A 1g , but also one additional (E g ) mode in calcite [2], respectively two further modes (B 1g and B 2g ) in aragonite [9], are the SRSpromoting vibration modes in these crystals. Here, the question arises, whether a carbonate crystal structure with a very different arrangement of [CO 3 2 Crystallography Crystals of Pb 2 CO 3 Cl 2 , known also as mineral phosgenite, can be found occasionally as fine specimen in nature.…”

“…In recent investigations of stimulated Raman scattering and Raman induced four-wave mixing (RFWM) processes in crystals of the carbonate family, namely calcite (trigonal CaCO 3 ) [1,2] (but see also earlier work [3][4][5][6][7][8]), aragonite (orthorhombic CaCO 3 ) [9] and cerussite (PbCO 3 ) [10], these crystals turned out to offer several attractive manifestations of nonlinear laser interactions, such as broadband frequency comb generation, cascaded and cross-cascaded χ (3) ↔ χ (3) interactions or self-upconversion via parametric four-wave processes. In all these investigations natural crystals had been used due to the substantial experimental difficulties to grow large high quality single crystals of these compounds.…”

“…b) Measurement accuracy ± 0.0003 μm. was observed at room temperature using an experimental set-up as described in detail in several earlier studies of SRS-active carbonates, see [1,2] for calcite, CaCO 3 , [9] for aragonite, CaCO 3 , and [10] for cerussite, PbCO 3 , with slight modifications of the registration part of the set-up, see Fig. 3.…”