There are only a few commercially available nonlinear optical materials in the spectral window of 3-20 μm, creating technological gaps that require new materials to address them. Alkali-metal chalcoarsenates (AAsQ2) are a promising class because of their high second harmonic generation (SHG) coefficients with γ-NaAsSe2(d33 = 169 pm/V) and β-LiAsS2(d33 = 98 pm/V). The AAsQ2 (A = Li, Na and Q = S, Se) compounds are made up of 1-dimensional (1/∞)[AQ2]— chains, connected by pyramidal AQ3 units as observed in the two structures. The chains are parallel and engage in inter-chain interactions via long As···Se contacts. γ-NaAsSe2 (Pc) undergoes a phase transition to the centrosymmetric δ-NaAsSe2 (Pbca) upon melting, making it a challenge to grow large single crystals for NLO applications. Here we report the crystal growth of γ-NaAsSe2 and β-LiAsS2 used for single crystal SHG measurements. We studied the structural effects of substituting with Na atoms with K in γ-NaAsSe2.
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