Regulating off-centering distortion maximizes photoluminescence in halide perovskites
Regulating off-centering distortion maximizes photoluminescence in halide perovskites作者机构：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
出 版 物：《National Science Review》 (国家科学评论(英文版))
年 卷 期：2021年第8卷第9期
页 面：60-67页
核心收录：
学科分类：08[工学] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）]
基 金：supported by the National Natural Science Foundation of China (51527801, U1930401 and 17N1051-0213) supported by the the US Department of Energy (DOE),Office of Science,Basic Energy Sciences,under Grant No. SC0012541 (samples synthesis and ambient properties characterization) supported by the the US Department of Energy,Office of Science,Basic Energy Sciences,under Contract No. DE-AC02–06CH11357 supported by the National Science Foundation (NSF)—Earth Sciences(EAR-1634415) Department of Energy Geo Sciences (DEFG02-94ER14466) partially by COMPRES through NSF Cooperative Agreement EAR-1661511 supported by DOE National Nuclear Security Administration under Award DE-NA0001974, with partial instrumentation funding by NSF Argonne National Laboratory under Contract DE-AC02-06CH11357 partially supported by the Laboratory Directed Research and Development program of Los Alamos National Laboratory (LANL) Triad National Security Administration of the US Department of Energy under contract number 89233218CNA000001 supported by a Tencent XPLORER Prize
主 题：halide perovskites high pressure off-centering distortion optical properties lone-pair electrons quantitative relationship
摘 要：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.
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