ABSTRACT Although possessing similar structural and electronic configurations with the tetrahedral nonlinear optical (NLO) active units, such as SO 4 , PO 4 and so on, the development of selenates with SeO 4 units have been long term hindered due to the lack of effective approaches to enhance polarizability and optical anisotropy. Here, a strategic integration between trigonal architecture construction and molecular polarization enhancement was proposed, which resulted in the discovery of an exceedingly performant selenate optical material, namely Hg 6 O 2 H(SeO 4 ) 3 I 3 ( HSOI ). This compound possess unique pseudo‐planar Hg 3 OI 3 secondary building units (SBUs), which formed the cloverleaf‐shaped layer and further construct the sandwich structure with the polar SeO 4 H FBUs inserted between the layers. Notably, HSOI exhibits an exceptionally large second harmonic generation (SHG) response (14.6×KDP), achieving a new record that is 170% higher than the previous value of nonlinear metal selenates. Meanwhile, a record high birefringence of selenates (∼ 0.2) was also achieved in HSOI . Theoretical calculations were carried out to reveal its optical origins and provide new insights for further structure‐driven functional materials design.
Li et al. (Tue,) studied this question.
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