Ultrastable, cationic three-dimensional lead bromide frameworks that intrinsically emit broadband white-light†,Chemical Science

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Ultrastable, cationic three-dimensional lead bromide frameworks that intrinsically emit broadband white-light†
Chemical Science ( IF 7.6 ) Pub Date : 2017-12-19 00:00:00 , DOI: 10.1039/c7sc04118g
Chengdong Peng ₁ , Zewen Zhuang ₁ , Huimin Yang ₁ , Guiyang Zhang ₁ , Honghan Fei ₁

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Herein, we report the unusual broadband white-light emission as an intrinsic property from two cationic lead bromide frameworks. This is the first time that the metal halide materials adopting a purely inorganic positively-charged three-dimensional (3D) topology have been synthesized, thus affording highly distorted Pb^II centers. The single-component white-light emitters achieve an external quantum efficiency of up to 5.6% and a correlated color temperature of 5727 K, producing typical white-light close to that of fluorescent light sources. Unlike the air/moisture-sensitive 3D organolead halide perovskites, our cationic materials are chemically “inert” over a wide range of pH as well as aqueous boiling condition. Importantly, these long-sought ultrastable lead halide materials exhibit undiminished photoluminescence upon continuous UV-irradiation for 30 days under atmospheric condition (∼60% relative humidity, 1 bar). Our mechanistic studies indicate the broadband emission have contributions from the self-trapped excited states through electron-vibrational coupling in the highly deformable and anharmonic lattice, as demonstrated by variable-temperature photoluminescence/absorption spectra as well as X-ray crystallography studies. The chemical robustness and structural tunability of the 3D cationic bromoplumbates open new paths for the rational design of hybrid bulk emitters with high photostability.

中文翻译：

超稳定的阳离子三维溴化铅框架，本质上发射宽带白光†

在此，我们将不寻常的宽带白光发射报告为两种阳离子溴化铅框架的固有特性。这是首次合成采用纯无机带正电三维（3D）拓扑的金属卤化物材料，从而提供高度扭曲的Pb ^II中心。单组分白光发射器的外量子效率高达 5.6%，相关色温为 5727 K，产生接近荧光光源的典型白光。与空气/湿度敏感的 3D 有机铅卤化物钙钛矿不同，我们的阳离子材料在广泛的 pH 值以及水沸腾条件下都具有化学“惰性”。重要的是，这些长期寻求的超稳定卤化铅材料在大气条件下（~60％相对湿度，1巴）连续紫外线照射30天后表现出不减弱的光致发光。我们的机理研究表明，宽带发射是通过高度变形和非谐晶格中的电子振动耦合而产生的自陷激发态的贡献，如变温光致发光/吸收光谱以及 X 射线晶体学研究所证明的那样。 3D 阳离子溴铅酸盐的化学稳定性和结构可调性为合理设计具有高光稳定性的混合体发射器开辟了新的途径。

更新日期：2017-12-19

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