Optically fine quality single crystals of pure thiourea (abbreviated as TU) CH 4 N 2 S and sodium acetatetrihydrate doped thiourea (abbreviated as STATH) NaC 3 H 13 N 2 SO 5 were effectively grown by slow evaporation method at room temperature from their aqueous solutions. The procured crystals were of average size 18×12×5 mm 3 (TU) and 17×8×5 mm 3 (STATH). Single and Powder X-ray Diffraction studies were consummated and the lattice specifications of the grown crystals have been assessed. Optical constants were appraised for both the samples by manipulating UV-Vis-NIR spectroscopy. Chemical composition of TU and STATH was scrutinized by EDX analysis. The dielectric response of both the samples was investigated in the frequency zone 100 Hz to 5 MHz besides solid state parameters were deliberated. The second harmonic generation (SHG) efficiency test manifests that STATH has the efficiency 1.506 times that of potassium dihydrogen phosphate (KDP).
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