Citation: Yuwei Kang, Can Yang, Jun Zhang, Qi Wu. Synergistic triple-site engineering in ABX₃-type hybrid halides for high-performance nonlinear optical crystals[J]. Chinese Chemical Letters, ;2026, 37(1): 111385. doi: 10.1016/j.cclet.2025.111385 shu

Synergistic triple-site engineering in ABX₃-type hybrid halides for high-performance nonlinear optical crystals

Yuwei Kang ^{a, b} ,
Can Yang ^a ,
Jun Zhang ^{c, *,} ,
Qi Wu ^{a, *,}

a.
State Key Laboratory of New Textile Materials and Advanced Processing Technologies, Wuhan Textile University, Wuhan 430200, China
b.
State Key Laboratory of Functional Crystals and Devices, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350108, China
c.
Key Laboratory of Functional Molecule Design and Interface Process, Anhui Jianzhu University, Hefei 230601, China

zhangjun@ahjzu.edu.cn

wuqi2011@whu.edu.cn

Received Date: 27 April 2025
Revised Date: 12 May 2025
Accepted Date: 28 May 2025
Available Online: 29 May 2025

Figures(4)

Achieving non-centrosymmetric (NCS) configurations in ABX₃-type hybrid halides remains a critical challenge for nonlinear optical (NLO) materials due to the conflicting requirements of high second-harmonic generation (SHG) response, wide bandgap, and phase-matching capabilities. Herein, we propose a triple-site modulation strategy by synergistically tailoring the A-site cations (2-methylimidazole cation/1-ethyl-3-methylimidazole cation), B-site metals (Sn²⁺/Pb²⁺), and X-site halogens (Cl/Br), which effectively disrupts lattice symmetry and enables NCS crystallization. Our results demonstrate a strong SHG response, an expanded optical bandgap and increased birefringence. The optimized compound C₆H₁₁N₂PbCl₃ exhibits a moderately strong SHG efficiency of 3.8 × KDP, a wide bandgap (3.87 eV), and enhanced birefringence (0.139@1064 nm), surpassing majority hybrid NLO materials. The innovative anionic framework introduced here broadens the scope of hybrid NLO crystals, facilitating the integration of various aromatic heterocyclic cations. This research provides a robust strategic framework for the development of advanced NLO materials.
- Nonlinear,
- Optical organic-inorganic hybrid,
- ABX₃ lone pair,
- Optimized balance
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Synergistic triple-site engineering in ABX3-type hybrid halides for high-performance nonlinear optical crystals

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通讯作者: 陈斌, bchen63@163.com

Synergistic triple-site engineering in ABX₃-type hybrid halides for high-performance nonlinear optical crystals