Nonlinear optical (NLO) crystals are indispensable for the solid-state lasers for their ability to expand wavelength spectral to the regions where the directing lasing is difficult or even impossible, yet the rational design of a high-performance NLO crystal remains a great challenge owing to the severe structural and properties' requirements. Herein, a new noncentrosymmetric (NCS) and polar gallium iodate, LiGa(IO ) , with a novel 2D anionic layer, is successfully designed and synthesized by the aliovalent substitution strategy based on classic α-LiIO . The 2D [Ga(IO ) ] layer in LiGa(IO ) is built from the GaO octahedra and highly polarizable units IO . Compared with its parent compound, the partial replacement of A-site Li cation with main group Ga cation facilitates LiGa(IO ) to possess excellent NLO properties, including the large second-harmonic generation (SHG) response (14 × KH PO (KDP) @ 1064 nm), wide bandgap (4.25 eV), large birefringence (0.23 @ 1064 nm), and wide optical transparency from UV to mid-IR. These reveal that LiGa(IO ) will be a promising NLO crystal.
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