The search for new IR nonlinear optical (NLO) materials is a very active field in modern Inorganic Materials Chemistry. By applying a research strategy that combines “structural design” with “exploratory synthesis”, we have discovered a number of new IR NLO materials, namely the BaGa₄Se₇, LiGaGe₂Se₆, Li₂In₂MQ₆ (M=Si,Ge; Q = S,Se), and BaGa₂MQ_6⁽M = Si,Ge;Q = S,Se) compounds. They possess not only large NLO responses and large band gaps but also the valuable thermal behavior of congruent-melting, which makes it feasible to grow high quality bulk crystals needed for thorough evaluation and practical application. We have obtained high quality BaGa₄Se₇ single crystal in centimeter size and measured many important physical properties incluing the refractive index, the NLO coeffecient, and the laser damage threshold. The results indicate that BaGa₄Se₇ is a promising new IR NLO material with good overall properties.

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