Optoelectronic Dichotomy of Mixed Halide CH3NH3Pb(Br1-xClx)3 Single Crystals: Surface versus Bulk Photoluminescence

被引:21
作者
Li, Zhongguo [1 ]
Kolodziej, Charles [1 ]
Zhang, Taiyang [2 ]
McCleese, Christopher [1 ]
Kovalsky, Anton [1 ]
Zhao, Yixin [2 ]
Lambrecht, Walter R. L. [3 ]
Burda, Clemens [1 ]
机构
[1] Case Western Reserve Univ, Dept Chem, Cleveland, OH 44106 USA
[2] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, Shanghai 200240, Peoples R China
[3] Case Western Reserve Univ, Dept Phys, Cleveland, OH 44106 USA
基金
中国国家自然科学基金;
关键词
METHYLAMMONIUM LEAD IODIDE; HIGH-PERFORMANCE; PEROVSKITES; CARRIERS; BANDGAP; LENGTHS; PASSIVATION; TRANSPORT; INTERPLAY;
D O I
10.1021/jacs.8b07560
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In this work, the spatially dependent recombination kinetics of mixed-halide hybrid perovskite CH3NH3Pb-(Br1-xClx)(3) (0 <= x <= 0.19) single crystals are investigated using time-resolved photoluminescence spectroscopy with one- and two-photon femtosecond laser excitation. The introduction of chloride by substituting a fraction of the bromide leads to a decreased lattice constant compared to pure bromide perovskite (x = 0) and a higher concentration of surface defects. The measured kinetics under one-photon excitation (1PE) shows that increasing the chloride addition quenches the photoluminescence (PL) lifetimes, due to substitution-induced surface defects. In stark contrast, upon 2PE, the PL lifetimes measured deeper in the bulk become longer with increasing chloride addition, until the halide substitution reaches the critical concentration of similar to 19%. At x = 19% Cl concentration, a significant reversal of this behavior is observed indicating a change in crystal structure beyond the continuous trends observed at lower percentages of halide substitution (x <= 11%). The observed opposing trends, based on 1PE versus 2PE, highlight a dichotomy between extrinsic (surface) and intrinsic (bulk) effects of chloride substitution on the carrier dynamics in lead bromide perovskites. We discuss the physical relation between halide exchange and bulk carrier lifetimes in CH3NH3PbBr3 in terms of the Rashba effect. We propose that the latter is suppressed at the surface due to disorder in the alignment of the MA and that it increases in the bulk with Cl concentration because of the reduction in lattice parameters, which compresses the space available for the MA orientational degrees of freedom.
引用
收藏
页码:11811 / 11819
页数:9
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