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Stepwise Substitution Strategy for Beryllium-Based Selenites with Enhanced SHG Response, Moderate Birefringence, and Short UV Cutoff Edges

Yurui Wang,Xuehua Dong,Wei Zeng,Ling Huang,Zhien Lin,Hongmei Zeng,Guohong Zou

Designing nonlinear optical (NLO) materials that simultaneously exhibit enhanced second-harmonic generation (SHG), moderate birefringence (Δn), and short-wavelength ultraviolet (UV) transparency remains a significant challenge. This study presents a stepwise structural regulation strategy using the International Zeolite Association (ABW)-type zeolite NH4BePO4 (I) as the parent material. By systematically modulating the anionic units, we successfully synthesized two compounds: KBe2(HPO3)2F (II) and NH4Be2(OH)(SeO3)2·H2O (III). Compound III represents a breakthrough, demonstrating an SHG intensity 4.0 times greater than that of KH2PO4, a birefringence of 0.080 at 546 nm, and a UV cutoff at 203 nm. The enhanced optical anisotropy and NLO efficiency of compound III arise from the stereochemically active lone pairs in the [SeO3] groups. By optimizing SHG intensity, short-wavelength UV transparency, and birefringence simultaneously, compound III addresses the key challenge of designing high-performance short-wavelength UV NLO materials. This work not only validates the stepwise regulation strategy but also provides a design framework for achieving balanced NLO performance, paving the way for the development of next-generation optical materials.