Reticular chemistry-aided effective design of new second-order nonlinear optical selenites.

IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Materials Horizons Pub Date : 2024-10-09 DOI:10.1039/d4mh01043d
Qian Li, Yi Zheng, Hongping Wu, Zhanggui Hu, Jiyang Wang, Yicheng Wu, Hongwei Yu
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Abstract

Noncentrosymmetric (NCS) compounds are particularly important for modern optoelectronic technology, yet their rational structural design remains a great challenge. Herein, assisted by the idea of bottom-up reticular chemistry, seven new NCS selenites, AM3[SeO3]2[Se2O5]3 (A = K+/Rb+/Cs+; M = Al3+/Ga3+/In3+), have been successfully designed and synthesized by assembling main-group metal octahedral units and SeO3 units, to construct honeycomb layers with regular channels to accommodate a variety of cations, and using planar hexagonal shapes to orientate the groups within the network. Based on this strategy, the overall symmetry of the solid-state compounds was effectively controlled, and by modifying locally connected atoms or groups, without disrupting the overall prototypical framework, a series of iso-reticular analogues have been obtained, which greatly increases the probability of NCS structures. Three of these compounds, CsM3[SeO3]2[Se2O5]3 were characterized experimentally and theoretically. The results show that they all have moderate second harmonic generation (SHG) responses, which are as large as that of commercial KH2PO4, and wide band gaps. Our study confirms the feasibility of reticular chemistry-assisted strategy in designing nonlinear optical materials with stable frameworks and good performance.

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网状化学辅助有效设计新型二阶非线性光学硒化物。
非半对称性(NCS)化合物对于现代光电技术尤为重要,然而合理的结构设计仍然是一项巨大的挑战。在此,我们利用自下而上的网状化学思想,通过组装主族金属八面体单元和 SeO3 单元,构建具有规则通道的蜂窝层以容纳各种阳离子,并利用平面六边形来定向网络内的基团,成功设计和合成了七种新型非新对称硒化物 AM3[SeO3]2[Se2O5]3(A = K+/Rb+/Cs+;M = Al3+/Ga3+/In3+)。基于这种策略,固态化合物的整体对称性得到了有效控制,通过改变局部相连的原子或基团,在不破坏整体原型框架的情况下,获得了一系列等距类似物,从而大大提高了 NCS 结构的概率。对其中的三种化合物 CsM3[SeO3]2[Se2O5]3 进行了实验和理论表征。结果表明,它们都具有适度的二次谐波发生(SHG)响应,与商用 KH2PO4 的响应一样大,并且具有宽带隙。我们的研究证实了网状化学辅助策略在设计具有稳定框架和良好性能的非线性光学材料方面的可行性。
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来源期刊
Materials Horizons
Materials Horizons CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
18.90
自引率
2.30%
发文量
306
审稿时长
1.3 months
期刊介绍: Materials Horizons is a leading journal in materials science that focuses on publishing exceptionally high-quality and innovative research. The journal prioritizes original research that introduces new concepts or ways of thinking, rather than solely reporting technological advancements. However, groundbreaking articles featuring record-breaking material performance may also be published. To be considered for publication, the work must be of significant interest to our community-spanning readership. Starting from 2021, all articles published in Materials Horizons will be indexed in MEDLINE©. The journal publishes various types of articles, including Communications, Reviews, Opinion pieces, Focus articles, and Comments. It serves as a core journal for researchers from academia, government, and industry across all areas of materials research. Materials Horizons is a Transformative Journal and compliant with Plan S. It has an impact factor of 13.3 and is indexed in MEDLINE.
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