卤化物
激子
金属卤化物
二次谐波产生
共振(粒子物理)
材料科学
光子学
激发态
化学
化学物理
光电子学
无机化学
原子物理学
物理
凝聚态物理
激光器
光学
作者
Peng Cheng,Xiaodi Jia,Siqian Chai,Geng Li,Mingyang Xin,Junjie Guan,Xiaopeng Han,Han Wang,Shuming Zeng,Youquan Zheng,Jialiang Xu,Xian‐He Bu
标识
DOI:10.1002/anie.202400644
摘要
Chiral hybrid organic-inorganic metal halides (HOMHs) offer an ideal platform for the advancement of second-order nonlinear optical (NLO) materials owing to their inherent noncentrosymmetric structures. The enhancement of optical nonlinearity of chiral HOMHs could be achieved by matching the free exciton and/or self-trapped exciton energy levels with desired NLO frequencies. However, the current scarcity of resonance modes and low resonance ratio hamper the further improvements of NLO performance. Herein, we propose a new resonant channel of charge transfer (CT) excited states from metal halide polyhedra to organic ligand to boost the second-order optical nonlinearity of chiral HOMHs. The model lead halide (C7H10N)PbBr3 (C7H10N=1-ethylpyridinium) exhibits a drastically enhanced second harmonic generation in resonance to the deep CT exciton energy, with intensity of up to 111.0 times that of KDP and 10.9 times that of urea. The effective NLO coefficient has been determined to be as high as ~40.2 pm V-1, balanced with a large polarization ratio and high laser damage threshold. This work highlights the contribution of organic ligands in the construction of a resonant channel for enhancing second-order NLO coefficients of metal halides, and thus provides guidelines for designing new chiral HOMHs materials for advanced nonlinear photonic applications.
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