Citation: Yu Zhou, Lin-Tao Jiang, Xiao-Ming Jiang, Bin-Wen Liu, Guo-Cong Guo. Mixed-anion square-pyramid [SbS₃I₂] units causing strong second-harmonic generation intensity and large birefringence[J]. Chinese Chemical Letters, ;2025, 36(4): 109740. doi: 10.1016/j.cclet.2024.109740 shu

Mixed-anion square-pyramid [SbS₃I₂] units causing strong second-harmonic generation intensity and large birefringence

Yu Zhou ^{a, c} ,
Lin-Tao Jiang ^{a, c} ,
Xiao-Ming Jiang ^{a, b} ,
Bin-Wen Liu ^{a, b, *,} ,
Guo-Cong Guo ^{a, b, *,}

a.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
b.
Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350002, China
c.
College of Chemistry, Fuzhou University, Fuzhou 350116, China

bwliu@fjirsm.ac.cn

gcguo@fjirsm.ac.cn

Received Date: 19 January 2024
Revised Date: 27 February 2024
Accepted Date: 6 March 2024
Available Online: 8 March 2024

Figures(3)

Enhancement of the nonlinear optical (NLO) output power of lasers requires urgent development of an NLO crystal with a significant second-harmonic generation (SHG) response and sufficient birefringence for phase-matching capability; however, simultaneously optimizing these two key parameters remains a great challenge. In contrast to traditional single-anion units, the stereochemically-active lone pair Sb³⁺ ion is coordinated by S²⁻ and I⁻ ions to yield the mixed-anionic SbSI chalcohalide that can enhance hyperpolarizability and anisotropic polarizability concurrently. As anticipated, SbSI exhibited the largest SHG response (5.7 × AgGaS₂@1.91 µm) among phase-matching Sb-based sulfides, the favorable laser-induced damage threshold (LIDT, 2.3 × AgGaS₂@2.09 µm), and the giant calculated birefringence (0.62@1.91 µm). Structural analysis and computational simulations indicate that the highly polarizable mixed anion determine the enormous SHG response and birefringence.
- Chalcohalide,
- Mixed-anionic units,
- Nonlinear optical,
- Birefringence,
- Structure-property relationship
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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

Mixed-anion square-pyramid [SbS3I2] units causing strong second-harmonic generation intensity and large birefringence

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通讯作者: 陈斌, bchen63@163.com

Mixed-anion square-pyramid [SbS₃I₂] units causing strong second-harmonic generation intensity and large birefringence