Citation: Xiantan Lin, Yicong Lv, Xiaoqi Li, Zengshan Yue, Kai Li, Qingyin Wei, Qianxi Wang, Junhua Luo, Xitao Liu. Rational design of a high-efficiency lead halide organic-inorganic hybrid nonlinear optical switch via molecular engineering[J]. Chinese Chemical Letters, ;2026, 37(7): 111083. doi: 10.1016/j.cclet.2025.111083 shu

Rational design of a high-efficiency lead halide organic-inorganic hybrid nonlinear optical switch via molecular engineering

Xiantan Lin ^{a, b} ,
Yicong Lv ^{a, b} ,
Xiaoqi Li ^{a, c} ,
Zengshan Yue ^a ,
Kai Li ^a ,
Qingyin Wei ^a ,
Qianxi Wang ^a ,
Junhua Luo ^{a, c, *,} ,
Xitao Liu ^{a, c, *,}

a.
State Key Laboratory of Functional Crystals and Devices, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
b.
College of Chemistry and Materials Science, Fujian Normal University, Fuzhou 350007, China
c.
Fujian College, University of Chinese Academy of Sciences, Fuzhou 350002, China

jhluo@fjirsm.ac.cn

xtliu@fjirsm.ac.cn

Received Date: 23 January 2025
Revised Date: 8 March 2025
Accepted Date: 12 March 2025
Available Online: 31 March 2025

Figures(5)

As an indispensable subset of functional materials, quadratic nonlinear optical (NLO) switches have garnered increasing attention owing to their vast potential in next-generation intelligent optoelectronic devices. Despite considerable progress in NLO switches based on solid-state phase transitions, identifying an effective strategy to design high-efficiency NLO switches remains a huge challenge. Herein, we present a molecular engineering approach to develop a high-efficiency lead halide organic-inorganic hybrid NLO switch, (C₈H₁₂N)₂Pb₂Cl₆·H₂O (NMPTPC). Through the substitution of hydrogen with a methyl group (-CH₃) in protonated N-methylaniline, the initial compound (C₇H₁₀N)₂Pb₂Cl₆·H₂O (NMAPC) transformed into NMPTPC retaining the original space group, which gives rise to a dramatic enhancement of second harmonic generation (SHG) and phase transition temperature. As expected, NMPTPC exhibits high-efficiency modulation of the SHG property (2.6 times that of KH₂PO₄) and a high phase transition temperature of 372 K. Notably, NMPTPC exhibits a remarkable temperature-dependent SHG behavior, with an impressive "ON/OFF" ratio of approximately 70, underscoring its significant potential as a high-efficient solid-state NLO switch. Based on in-depth crystal structure analysis and theoretical calculations, the modulation of the NLO property is attributed to the asymmetric distortion of the [PbCl₆]⁴⁻ octahedra coupled with π-conjugated aromatic amines with a large dipole moment. This research highlights a promising strategy for advancing the development of high-efficiency NLO switches and provides insights into their applications in next-generation intelligent optoelectronic devices.
- Nonlinear optical switch,
- Perovskite,
- Phase transition,
- Second harmonic generation,
- High-efficiency
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