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Temperature-dependent thermo-mechanical and Raman spectroscopy study of the SRS-active melilite-type crystal Ca2ZnSi2O7 (hardystonite) at its incommensurate–commensurate phase transition



Stimulated Raman scattering (SRS) active crystals of Ca2ZnSi2O7 (hardystonite) adopt a melilite-type structure at temperatures above ca. 402 K, while at ambient conditions they show a two-dimensionally incommensurate structure modulation. To study the influence of the incommensurability of the structure on SRS-based χ(3)-nonlinear lasing of the crystals temperature-dependent Raman spectroscopy investigations at the commensurate–incommensurate phase-transition and comparative SRS measurements in the high-temperature and in the low-temperature phase of Ca2ZnSi2O7 are reported. In addition, the commensurate–incommensurate phase transition is characterised by caloric and dilatometric measurements, and linear optical properties of the crystals are given.