Abstract
Nonlinear optical (NLO) crystals play a significant role in optoelectronic industry. Herein, a new NLO crystal, K(H2O)[KI][PbI(C4H4O4)], has been rationally obtained by tuning halide perovskite materials with 2-methylmalonate group. K(H2O)[KI][PbI(C4H4O4)] features that the highly distorted [PbO4I2] polyhedron with large hyperpolarizability and prominent polarizability anisotropy is served as a bifuntional unit. Remarkably, the distorted [PbO4I2] polyhedrons are aligned in an oriented arrangement that leads to the effective superposition of their microscopic second-order nonlinear susceptibilities and the enhancement of optical anisotropy. Notably, K(H2O)[KI][PbI(C4H4O4)] exhibits a strong phase-matching SHG response of 5.6 × KDP and a large birefringence (Δnobv. = 0.24@546 nm). Theoretical calculations elucidate that the strong SHG response and the large birefringence are predominantly attributed to the directional arrangement of the highly distorted [PbO4I2] polyhedrons. Our discovery provides an effective path for the rational exploration of high-performance NLO crystals.
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