Designing Polar Covalent Hybrid Cadmium-Based Chalcohalides Ultraviolet Nonlinear Optical Crystal with Strong Optical Anisotropy via Double-Site Dual FBUs Tailoring

IF 13 2区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Small Pub Date : 2025-01-26 DOI:10.1002/smll.202412173

Yi-Fan Fu, Wen-Dong Yao, Jiajing Wu, Qiao-Feng Huang, Yu-Mei Zhang, Wenfeng Zhou, Wenlong Liu, Sheng-Ping Guo

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Abstract

The pressing demand for both established and innovative technologies to expand laser wavelengths has rendered high-performance nonlinear optical (NLO) crystals with large optical anisotropy indispensable. Here, centrosymmetric [SHC(NH₂)₂]₂CdBr₄ (1) and pseudo-2D layered [SC(NH₂)₂]₂CdBr₂ (2), as well as pseudo-3D noncentrosymmetric [SC(NH₂)₂]₂CdCl₂ (3) are successfully synthesized through the introduction of π-conjugated SC(NH₂)₂ groups. Compared to ionic compound 1 containing full-halogen coordination tetrahedra, covalent compounds 2 and 3 featuring novel polar [SC(NH₂)₂]₂CdX₂ (X = Br, Cl) tetrahedral units demonstrate enhanced bandgaps (>4 eV) and birefringences (>0.3@546 nm) due to the unique coordination environment. Remarkably, 3 exhibits a strong second-harmonic generation (SHG) response (2.1 × KH₂PO₄(KDP)), high laser-induced damage thresholds (30 × AgGaS₂(AGS), and excellent water stability. The birefringence of 3 is the largest among the hybrid halides NLO crystals containing d¹⁰ metal cations. Detailed theoretical calculations confirm that such a modified double-site dual functional building units (FBUs) substitution is an effective strategy for designing superior optical materials with large birefringence and strong SHG response, paving the way for the development of high-performance devices in related fields.

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通过双位点双 FBUs 裁剪设计具有强光学各向异性的极性共价杂化镉基卤化物紫外非线性光学晶体

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来源期刊

Small 工程技术-材料科学：综合

CiteScore

17.70

自引率

3.80%

发文量

1830

审稿时长

2.1 months

期刊介绍： Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments. With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology. Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.