In the present research work, the FT-IR, FT-Raman spectra of the Bis(thiourea) Cadmium chloride (BTCC) were recorded. The observed fundamental frequencies in finger print and functional group regions were assigned according to their uniqueness region. The computational calculations were carried out by HF and DFT (B3LYP, CAM – B3LYP, B3PW91 and MPW1PW91) methods with 3-21 G(d, p) basis set and the corresponding results were tabulated. The present compound is an organo-metallic compound which is made up of covalent and coordination covalent bonds and the modified vibrational pattern of the complex molecule associated with ligand group was analyzed. Moreover, 13C NMR and 1H NMR were calculated by using the gauge independent atomic orbital (GIAO) method with B3LYP methods and the 6-311++G(d,p) basis set and their spectra were simulated and the chemical shifts linked to TMS were compared. A study on the electronic and optical properties; absorption wavelengths, excitation energy, dipole moment and frontier molecular orbital energies were carried out. The kubo gap of the present compound was calculated related to HOMO and LUMO energies which confirm the occurring of charge transformation between the base and ligand. Besides frontier molecular orbitals (FMO), molecular electrostatic potential (MEP) was performed. The NLO properties related to Polarizability and hyperpolarizability based on the finite-field approach were also discussed. A new semiorganic nonlinear optical crystal of Bis(thiourea) Cadmium chloride (BTCC) was grown successfully by slow evaporation technique using water as solvent. The lattice parameters of the grown crystal have been determined by X-ray diffraction studies. Vibrational spectrum is recorded to determine symmetries of molecular vibrations. The recording of Optical absorbance spectrum revealed that this crystal has good transparency in the visible region. The nonlinear nature of the present crystal has been confirmed by the SHG test. Vickers micro-hardness test has done on the crystal and this shows that the crystal has greater physical strength.
