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An organic–inorganic hybrid polyiodate, namely, [o‐C5H4NHOH]2[I7O18(OH)]⋅3 H2O (I), featuring a novel branched polyiodate chain has been obtained by evaporation method. [o‐C5H4NHOH]2[I7O18(OH)]⋅3 H2O (I) crystalizes in the polar space group Ia and features an [I7O18(OH)]∞2- branched polyiodate chain in which [I3O9]3− trimers are grafted on the same side of the one‐dimensional (1D) chain based on [I4O11(OH)]3− tetramers. The asymmetric organic amine groups are beneficial to the polymerization of iodate groups and inducing the formation of the non‐centrosymmetric (NCS) structure. Compound I exhibits a rather large Second‐Harmonic‐ Generation (SHG) signal of 8.5×KH2PO4 (KDP) upon 1064 nm laser radiation, a moderate band gap of 3.90 eV and a high laser‐induced‐damage‐threshold (LIDT) of 182.34 MW cm−2, hence it is a promising new SHG material. The relationship between the structures of the organic amine groups and the overall structures has been also analyzed. [ABSTRACT FROM AUTHOR]

The first alkali‐metal vanadium iodate fluoride, CsVO2F(IO3), with a novel 3D anionic framework, has been rationally designed and hydrothermally synthesized. The 3D [VO2F(IO3)]− framework in CsVO2F(IO3) is built from 0D Λ‐shaped cis‐[VO3F(IO3)2]4− polyanions via corner‐sharing of oxo anions and bridging of the iodate groups. CsVO2F(IO3) displays both a strong second‐harmonic generation (SHG) 1.1 times as strong as KTiOPO4 (KTP) under 2.05 μm laser radiation and high laser‐induced damage threshold (LIDT) of 107.9 MW cm−2. This work provides a new route to design SHG crystals with stable 3D anionic structures from low‐dimensional structural building units. [ABSTRACT FROM AUTHOR]

A large nonlinear optical (NLO) coefficient and a wide band gap are two crucial but contradictory parameters that are difficult to achieve simultaneously in a single infrared (IR) NLO compound. A salt‐inclusion chalcogenide (SIC), Li[LiCs2Cl][Ga3S6] (1), was prepared that presents a nanosized tunnel framework constructed from monotype chalcogenide tetrahedra. Highly oriented covalent GaS4 tetrahedra in the host lead to a moderate second harmonic generation response (0.7 AgGaS2), and ionic guests effectively broaden the band gap to the widest value (4.18 eV) among all IR NLO chalcogenides, thereby achieving a remarkable balance between NLO efficiency and band gap. [ABSTRACT FROM AUTHOR]