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Article Abstract
Oxyhalides are promising candidates for nonlinear optical (NLO) applications due to their unique structural and optical properties. In this study, we report the synthesis of two tellurium-based oxyhalides, TeOCl and TeOCl, which exhibit distinct structural features and exceptional optical performance. TeOCl crystallizes in a noncentrosymmetric 2D layered structure, while TeOCl adopts a centrosymmetric 1D chain arrangement. Both compounds display wide optical transmission windows (0.30/0.31-25 μm), with TeOCl achieving a large second-harmonic generation (SHG) efficiency surpassing conventional materials and a significant birefringence (Δ = 0.185 at 546 nm). The SHG response of TeOCl is attributed to the alignment of nonlinear-active units driven by the [TeOCl] disphenoid and the stereochemically active lone pairs (SCALPs), facilitated by halogen-mediated structural distortion. These results highlight the potential of halogen modification for the design of advanced NLO materials with enhanced performance.
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