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Regulating off-centering distortion maximizes photoluminescence in halide perovskites

National Science Review 2021年第9期8卷 60-67页

作者： Xujie Lu Constantinos Stoumpos Qingyang Hu Xuedan Ma Dongzhou Zhang Songhao Guo Justin Hoffman Kejun Bu Xiaofeng Guo Yingqi Wang Cheng Ji Haijie Chen Hongwu Xu Quanxi Jia Wenge Yang Mercouri G.Kanatzidis Ho-Kwang Mao Center for High Pressure Science and Technology Advanced Research Department of Chemistry Northwestern University Department of Materials Science and Technology Voutes Campus University of Crete Center for Nanoscale Materials Argonne National Laboratory Partnership for Extreme Crystallography University of Hawaii at Manoa Department of Chemistry and Alexandra Navrotsky Institute for Experimental Thermodynamics Washington State University Earth and Environmental Sciences Division Los Alamos National LaboratoryLos Alamos Department of Materials Design and Innovation University at Buffalo The State University of New York

Metal halide perovskites possess unique atomic and electronic configurations that endow them with high defect tolerance and enable high-performance photovoltaics and optoelectronics. Perovskite light-emitting diodes have achieved an external quantum efficiency of over 20%. Despite tremendous progress,fundamental questions remain, such as how structural distortion affects the optical properties. Addressing their relationships is considerably challenging due to the scarcity of effective diagnostic tools during structural and property tuning as well as the limited tunability achievable by conventional methods. Here,using pressure and chemical methods to regulate the metal off-centering distortion, we demonstrate the giant tunability of photoluminescence (PL) in both the intensity (>20 times) and wavelength(>180 nm/GPa) in the highly distorted halide perovskites [CH3NH3GeI3, HC(NH2)2GeI3, and Cs Ge I3].Using advanced in situ high-pressure probes and first-principles calculations, we quantitatively reveal a universal relationship whereby regulating the level of off-centering distortion towards 0.2 leads to the best PL performance in the halide perovskites. By applying this principle, intense PL can still be induced by substituting CH3NH~3+with Cs~+to control the distortion in (CH3NH3)1-xCsxGeI3, where the chemical substitution plays a similar role as external pressure. The compression of a fully substituted sample of CsGe I3further tunes the distortion to the optimal value at 0.7 GPa, which maximizes the emission with a10-fold enhancement. This work not only demonstrates a quantitative relationship between structural distortion and PL property of the halide perovskites but also illustrates the use of knowledge gained from high-pressure research to achieve the desired properties by ambient methods.

关键词： halide perovskites high pressure off-centering distortion optical properties lone-pair electrons quantitative relationship

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