Over the last few decades, the development of each new nonlinear optical (NLO)-active functional unit has led to the discoveries of a series of excellent NLO materials. In the present work, based on first-principles studies, we identified a novel deep-UV (DUV) NLO-active functional unit, a non-π-conjugated group viz. (NH2 SO3 )- . By combining alkaline-earth metals with (NH2 SO3 )- group, two DUV transparent NLO sulfamates, M(NH2 SO3 )2 (M=Sr, Ba) with superior optical properties including strong SHG responses (1.2 and 2.7 × KH2 PO4 (KDP)), short UV cut-off edge (<190 nm) and moderate birefringence (0.056@589.3 nm for Sr(NH2 SO3 )2 ) were successfully synthesized. Our work has provided not only two promising DUV transparent NLO crystals, but also an innovative non-π-conjugated unit for developing more DUV transparent NLO materials.
Keywords: DUV; first-principles studies; nonlinear optical crystals; second harmonic generation; sulfamates.
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