Intermolecular Hydrogen-Bonding Correlated Structure Distortion and Broadband White-Light Emission in 5-Ammonium Valeric Acid Templated Lead Chloride Perovskites
Intermolecular Hydrogen-Bonding Correlated Structure Distortion and Broadband White-Light Emission in 5-Ammonium Valeric Acid Templated Lead Chloride Perovskites
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5-戊酸铵模板氯化铅钙钛矿中分子间氢键相关结构畸变和宽带白光发射
DOI：
10.1021/acs.cgd.1c00566
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发表时间：
2021-09
影响因子：
3.8
通讯作者：
He Yunbin
中科院分区：
文献类型：
--
作者：
Yang Wantian;Xiao Xinglin;He Huanfeng;Tong Guoliang;Hu Jiarui;Xiao Xingfu;Chen Junnian;Li Mingkai;He Yunbin
二维（2D）钙钛矿宽带发光体在发光领域获得了广泛的关注。但结构畸变调制的局限性阻碍了发光强度的提高，有机二胺的高毒性对人体健康造成潜在危害。本文利用绿色有机间隔基5-戊酸铵（Ava）模板化新型二维氯化铅杂化物Ava 2 PbCl 4，其中相邻有机阳离子层之间形成分子间O 1···H-O2相互作用。Ava 2 PbCl 4中的分子间氢键导致更大的阳离子渗透深度，这使得比五亚甲基二铵氯化铅（PDAPbCl 4）参比物更大的结构变形成为可能。这种八面体变形进一步导致Ava 2 PbCl 4中的超宽带发射，与PDAPbCl 4（0.4%）相比，其实现了增强的光致发光量子产率（2.83%）。进一步的机制研究表明，这些宽带发光可以归因于瞬态自陷激子发光。密度泛函理论计算表明，八面体畸变的电子起源。上述研究结果揭示了分子间氢键在调控二维钙钛矿结构中的重要作用，为设计用于光电应用的绿色钙钛矿结构提供了理论依据.
Two-dimensional (2D) perovskite broadband emitters are gaining intensive attention in light-emitting fields. However, the limitation of structure distortion modulation hinders the increase of emission intensity, and the high toxicity of organic diamine causes potential damage to human health. Herein, we utilize a green organic spacer 5-ammonium valeric acid (Ava) to template novel 2D lead chloride hybrids, Ava2PbCl4, where intermolecular O1···H–O2 interactions form between the adjacent organic cation layers. The intermolecular hydrogen bonding in Ava2PbCl4causes a larger cation penetration depth which enables larger structural deformation than the pentamethylenediammonium lead chloride (PDAPbCl4) reference. This octahedral deformation further leads to ultrabroadband emission in Ava2PbCl4, which achieves enhanced photoluminescence quantum yield (2.83%) compared to PDAPbCl4(0.4%). Further mechanism investigation indicates that these broadband emissions could be assigned as the transient self-trapped excitons luminescence. Density functional theory calculation indicates that the octahedral distortions are traced to an electronic origin as well. The above findings reveal the key role of intermolecular hydrogen bonding in modulating the photophysical properties of 2D perovskites and will benefit the design of green perovskites for optoelectronic applications.
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影响因子：
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