Alkali metals (Li, Na, K) doped anthracene high quality organic crystals were grown by slow evaporation at ambient environment. The relative occupancy of dopants and its influence of AN lattice phonons has been probed using elemental and diffraction analysis respectively. These alkali metal ions act as an efficient optically active sites, thereby projecting enhancement in UV region and photoluminescence studies. The nonlinear susceptibility (χ(3)) have been evaluated for doped crystals from Z ‐ scan technique and the values of these parameters found to be 10−2 esu which was higher than reported organic crystals. The incorporation of the alkali metal ions progressively alters melting point, overtone vibrational bands, mechanical strength and nonlinear optical properties for the grown crystals. The improved thermal, mechanical, linear and nonlinear optical properties of doped crystals make it as a better candidate for optoelectronic applications.
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