Study of nonlinear optical behaviour in pure and brilliant green dye-doped potassium aluminium sulfate dodecahydrate (KAS) single crystals
摘要
High-quality inorganic crystals play a crucial role in the advancement of modern photonic devices. In this communication, we report for the first time the growth and comprehensive characterisation of novel Brilliant Green (BG) dye-doped potassium aluminium sulfate dodecahydrate (KAS), denoted as BGDDKAS, single crystals. The crystals were successfully grown at room temperature by a low-cost slow evaporation solution growth technique using double-distilled water as the solvent. Optically transparent and good-quality pure KAS and BGDDKAS crystals with BG concentrations of 0.02 mol% and 0.04 mol% were harvested after growth periods of 26 and 32 days, respectively. Both as-grown single crystals and powdered samples were subjected to various characterisation techniques to examine the influence of BG dye incorporation on the structural, optical, and third-order nonlinear optical (TONLO) properties. Powder X-ray diffraction analysis revealed sharp and well-defined diffraction peaks, confirming the high crystalline quality of both pure and BGDDKAS crystals. Fourier-transform infrared (FTIR) spectroscopy evidenced the successful incorporation of BG dye into the KAS lattice through observable shifts in characteristic vibrational bands. UV–Visible spectral analysis in the wavelength range of 200–1000 nm was employed to determine the optical cut-off wavelengths and bandgap energies of pure and BGDDKAS crystals at room temperature. Photoluminescence studies indicated a reduction in microscopic defects such as vacancies and self-interstitials upon BG dye doping. The TONLO properties of pure KAS and BGDDKAS crystals were investigated using the Z-scan technique with a He–Ne laser operating at 632.8 nm. Key nonlinear optical parameters, including the nonlinear refractive index, nonlinear absorption coefficient, and third-order nonlinear susceptibility (χ3), were evaluated. The χ3 values were determined to be 3.52 × 10⁻⁶ esu for pure KAS, 4.92 × 10⁻⁶ esu for BGDDKAS1, and 5.97 × 10⁻⁶ esu for BGDDKAS2 crystals, demonstrating a significant enhancement in nonlinear optical response due to BG dye incorporation.