Abstract

AbstractAcquiring high‐performance ultraviolet (UV) nonlinear optical (NLO) materials that simultaneously exhibit a strong second harmonic generation (SHG) coefficients, as short as possible SHG phase‐matching (PM) wavelength and non‐hygroscopic properties has consistently posed a significant challenge. Herein, through multicomponent modification of KBe2BO3F2 (KBBF), an excellent UV NLO crystal, Mg(C3O4H2)(H2O)2, was successfully synthesized in malonic system. This material possesses a unique 2D NLO‐favorable electroneutral [Mg(C3O4H2)3(H2O)2]∞ layer, resulting in the rare coexistence of a strong SHG response of 3×KDP (@1064 nm) and short PM wavelength of 200 nm. More importantly, it exhibits exceptional water resistance, which is rare among ionic organic NLO crystals. Theoretical calculations revealed that its excellent water‐resistant may be originated from its small available cavity volumes, which is similar to the famous LiB3O5 (LBO). Therefore, excellent NLO properties and stability against air and moisture indicate it should be a promising UV NLO crystal.

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