Experimental and computational studies of linear and nonlinear optical (NLO) properties of (2E)-3-(5-bromo-2-thienyl)-1-(4-nitrophenyl)prop-2-en-1-one (5B2SNC) single crystals are reported. Good-quality and large-sized single crystals of 5B2SNC were successfully grown and characterized by powder X-ray diffraction and high-resolution X-ray diffractometry techniques. 5B2SNC was found to crystallize in the monoclinic noncentrosymmetric space group Cc and possesses moderately good crystalline perfection. The linear optical properties were investigated using the absorption spectrum, which reveals a direct optical band gap of 3.1 eV. The thermal stability was studied with thermogravimetric analysis/differential thermal analysis. The powder second harmonic generation efficiency was evaluated by the Kurtz and Perry method, and 5B2SNC was found to be 26 times more efficient than urea standard. Third-order NLO properties were studied by the z-scan technique with a femtosecond laser. The second hyperpolarizability was obtained to be ∼1.45 × 10−31 e.s.u. The molecule reveals a strong reverse saturation absorption and negative nonlinear refraction. The molecule exhibited good optical limiting properties, and its limiting threshold was measured to be ∼3.2 mJ cm−2. In addition, static electric dipole moments, linear polarizabilities, and first- and second-order hyperpolarizabilities were calculated by density functional theory (DFT). Highest occupied molecular orbital/lowest unoccupied molecular orbital band gaps were also evaluated by DFT calculations. The experimental and theoretical results showed that 5B2SNC exhibits excellent second- and third-order nonlinear optical properties.
