In this paper, an organic 4-nitroaniline picrate (4NP) single crystal was grown by solution growth method. Single crystal X-ray diffraction study revealed that grown crystal belongs to orthorhombic system with Pbcn space group. The solid state constants such as plasma energy, Penn gap, Fermi energy and polarizability of 4NP crystal were determined theoretically. The functional groups of the grown crystals were confirmed qualitatively from FTIR spectral analysis. The thermal decomposition and melting point of the crystal were determined from thermogravimetric analysis. The optical absorption and cut-off wavelength of the crystal were determined from UV-visible study. The second harmonic generation (SHG) efficiency of the grown crystal was measured by Kurtz–Perry SHG test using Nd : YAG laser. The laser damage threshold value of the grown crystal was estimated by multi-shot method using 1064 nm laser.

4-Bromoanilinium 4-methylbenzenesulfonate (4BPTS) single crystal was successfully grown from ethanol by slow evaporation method at room temperature. The structure of grown crystal was confirmed by single crystal X-ray diffraction studies. The presence of functional groups of grown crystal was confirmed by the Fourier transform infrared spectroscopy (FTIR) spectral analysis. UVVisible absorption study was performed on the grown crystal to determine the cut-off wavelength. The thermal stability of the grown crystal was investigated from the Thermogravimetric analysis (TGA)/ Differential thermal analysis (DTA) analysis. The mechanical behaviour of grown crystal was studied by using Vicker's microhardness test. The third order non-linear optical properties of 4BPTS were investigated by Z-scan technique with He-Ne laser radiation and the corresponding non-linear refractive index and absorption coefficients were also calculated.