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The nonlinear optical crystals of cobalt (Co 2+) mixed copper mercury thiocyanate have been grown by slow evaporation method using water and ethanol as solvents. The grown crystals have been subjected to different characterization analyses and the results were compared with pure copper mercury thiocyanate crystal (CMTC), which has been already reported. The single crystal X-ray diffraction shows that the addition of metallic impurity does not alter the basic structure of the parent crystal, but increases the cell volume markedly. The presence of functional groups has been identified using FT-IR analysis. Further the grown crystal is characterized by optical transmission analysis and thermal analysis. The thermal stability of the grown crystal is high, compared to pure CMTC crystal. The optical transparency of the grown crystal is studied by UV-Vis-NIR analysis. This study reveals that Co 2+ mixed CMTC crystal has wider transparent waveband than pure CMTC crystal. The relative second harmonic generation efficiency of the Co 2+ mixed CMTC crystal has been tested by Kurtz-Perry powder technique.

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