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Published on: December 29, 2016
Stereochemically Active Lone-Pair Containing Metal Substitution in Polar Axis toward a Giant Phase-Matchable Optical
Yuanyu Yang1, Yan Xiao2, Bingxuan Li3
1Key Laboratory of Magnetic Molecules and Magnetic Information Material of Ministry of Education, School of Chemistry and Material Science, Shanxi Normal University, Taiyuan 030031, China.
Abstract:
Atoms in special lattice sites can play a crucial role in realizing materials properties, which is long pursued but difficult to control. Herein, by adopting a stereochemically active lone-pair-containing metal substitution strategy, a nonlinear-optical (NLO) silicate crystal Li3(OH)PbSiO4 was successfully synthesized, featuring [PbSiO4]∞ layers with the perfect orientation of the stereochemically active lone-pair Pb(II) cation in the polar-axis lattice. Li3(OH)PbSiO4 overcomes the long-standing problem of silicates, that is, poor nonlinear properties because it exhibits both the largest birefringence of 0.082 and the largest phase-matchable second-harmonic-generation (SHG) efficiency of 21 × KDP among the known silicates. The successful polar-axis lattice substitution could offer a new direction for realizing the rational control of materials structures and properties.
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