“…Thiourea molecule is attracting not only due to the structural chemistry but also the attainability of formation of semiorganic coordination complexes which results in enhanced NLO activity [14,15]. Thiourea based semiorganic optical crystals like potassium thiourea chloride (PTC) [16], calcium bis(thiourea) chloride (CBTC) [17], pure and magnesium doped ZTS [18], bis thiourea ammonium nitrate (BTAN) [19], cadmium thiourea acetate (CTA) [5], mono-thiourea cadmium sulfate dehydrate (MTCSD) [6] are good examples of engineering the materials with high nonlinearity out of an organic ligand with vanishing microscopic dipole moment (thiourea) by metal complexation, which exhibit very high NLO properties. Hence, our attention has been focused towards the development of semiorganic materials with thiourea ligand because of their interesting architecture and wide variety of applications.…”