Ba2[MoO3(OH)(IO3)2]IO3: A Promising SHG Material Featuring a Λ-Shaped Functional Motif Achieved by Universal Mono-Site Substitution

The first polar alkaline-earth metal molybdenum iodate, Ba-2[MoO3(OH)(IO3)(2)]IO3, with a Lambda-shaped [MoO3(OH)(IO3)(2)](3)(-) functional motif, was rationally designed. A zero-dimensional (OD) [MoO3(OH)(IO3)(2)](3-) unit is derived from OD [MoO2(OH)(IO3)(3)](2-) polyanion through anionic monosite substitution. Ba-2[MoO3(OH)(IO3)(2)]IO3 possesses a strong phase-matchable second-harmonic-generation (SHG) response of approximately 8 times that of benchmark KH2PO4 (KDP), a broad transparent spectral region from near-ultraviolet to mid-infrared (0.29-10.6 mu m), a large band gap of 3.78 eV, and a high laser-induced damage threshold (LDT) of 92.3 MW cm(-2). The results Particle Size (ern) suggest that Ba-2[MoO3(OH)(IO3)(2)]IO3 can be potentially applied in the mid-infrared nonlinear optical field. Theoretical calculations demonstrate that the large SHG response of the title compound originates mainly from the Lambda-shaped [MoO3(OH)(IO3)(2)](3-) functional unit. From multisite substitution to mono-site substitution, this work provides a more generic route to synthesize SHG materials.