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Strong Second- and Third-Harmonic Generation in 1D Chiral Hybrid Bismuth Halides
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2021-09-24 , DOI: 10.1021/jacs.1c06567
Li Yao 1 , Zhouxiaosong Zeng 2 , Chengkun Cai 1 , Peng Xu 3 , Honggang Gu 4 , Liang Gao 1 , Junbo Han 5 , Xiaowei Zhang 6 , Xi Wang 1 , Xiao Wang 2 , Anlian Pan 7 , Jian Wang 1 , Wenxi Liang 1 , Shiyuan Liu 1, 4, 5 , Chao Chen 1, 8 , Jiang Tang 1, 8
Affiliation  

Breaking the symmetry of a crystal structure can enable even-order nonlinear activities, including second-harmonic generation (SHG). The emerging chiral hybrid organic–inorganic metal halides feature unique optical and electronic properties and flexible crystal structures, making them a class of promising nonlinear optical materials. However, their nonlinear response performances are currently inferior to traditional nonlinear crystals, because of the lack of research on resonant enhancement and third-harmonic generation (THG). Herein, we designed chiral hybrid bismuth halides with naturally nonsymmetrical structure to enable SHG. Simultaneously, these chiral compounds preserve 1D crystal structures to create strong free exciton, broad self-trapped exciton (STE), and discrete band energy levels, which facilitate the resonant enhancement of SHG and THG susceptibilities. These new chiral films showcase superior effective SHG susceptibility (χ(2) ∼ 130.5 pm V–1 at an interesting wavelength of 1550 nm), exceeding that of the reference, a commercial LiNbO3(2) ∼ 83.4 pm V–1) single-crystal film. Furthermore, their THG intensities are even higher than their SHG intensities, with effective THG susceptibility (χ(3)) being ∼9.0 × 106 pm2 V–2 at 1550 nm (37 times that of the reference monolayer WS2). Their high SHG and THG performances indicate the promising future of these 1D chiral hybrid bismuth halides toward nonlinear optical applications.

中文翻译:

一维手性杂化卤化铋中的强二次和三次谐波产生

打破晶体结构的对称性可以实现偶数阶非线性活动,包括二次谐波生成 (SHG)。新兴的手性杂化有机-无机金属卤化物具有独特的光学和电子特性以及灵活的晶体结构,使其成为一类很有前途的非线性光学材料。然而,由于缺乏对共振增强和三次谐波产生(THG)的研究,它们的非线性响应性能目前不如传统的非线性晶体。在此,我们设计了具有自然非对称结构的手性杂化卤化铋以实现 SHG。同时,这些手性化合物保持一维晶体结构以产生强自由激子、宽自陷激子 (STE) 和离散带能级,这有助于增强 SHG 和 THG 磁化率的共振。这些新的手性薄膜展示了卓越的有效 SHG 磁化率(χ(2) ∼ 130.5 pm V –1在有趣的 1550 nm 波长下),超过了参考文献,商业 LiNbO 3(2) ∼ 83.4 pm V –1 ) 单晶膜。此外,它们的 THG 强度甚至高于它们的 SHG 强度,有效的 THG 磁化率(χ (3))在 1550 nm 处为 ~9.0 × 10 6 pm 2 V –2(参考单层 WS 2 的37 倍)。它们的高 SHG 和 THG 性能表明这些一维手性混合卤化铋在非线性光学应用中的前景广阔。
更新日期:2021-10-06
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