Short Aromatic Diammonium Ions Modulate Distortions in 2D Lead Bromide Perovskites for Tunable White-Light Emission

被引:25
作者
Fu, Ping [1 ,2 ]
Quintero, Michael A. [2 ]
Welton, Claire [3 ]
Li, Xiaotong [2 ]
Cucco, Bruno [4 ]
De Siena, Michael C. [2 ]
Even, Jacky [5 ]
Volonakis, George [4 ]
Kepenekian, Mikael [4 ]
Liu, Runze [1 ]
Laing, Craig C. [2 ]
Klepov, Vladislav [2 ]
Liu, Yukun [6 ]
Dravid, Vinayak P. [6 ]
Reddy, G. N. Manjunatha [2 ,3 ]
Li, Can [1 ]
Kanatzidis, Mercouri G. [2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[3] Univ Lille, Univ Artois, Cent Lille Inst, Un Catalyse & Chim Solide,CNRS,UMR 8181 UCCS, F-59000 Lille, France
[4] Univ Rennes, CNRS, Inst Sci Chim Rennes, INSA Rennes,ENSCR, F-35000 Rennes, France
[5] Univ Rennes, CNRS, Inst FOTON, INSA Rennes,UMR 6082, F-35000 Rennes, France
[6] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
基金
美国国家科学基金会; 欧盟地平线“2020”;
关键词
SOLID-STATE NMR; HALIDE PEROVSKITES; IODIDE PEROVSKITES; RUDDLESDEN-POPPER; SPACER; SEMICONDUCTORS; STABILITY; EVOLUTION; CATIONS; LAYERS;
D O I
10.1021/acs.chemmater.2c02471
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
White-light broadband emission in the visible range from the low-dimensional halide perovskites is commonly attributed to structural distortions in lead bromide octahedra. In this paper, we report Dion-Jacobson-phase two-dimensional (2D) lead bromide perovskites based on short aromatic diammonium cations, p-phenylene diammonium (pPDA), m-phenylene dia-mmonium (mPDA), and two 1D compounds templated by o-phenylene diammonium (oPDA). All of the compounds exhibit white-light emission. Single-crystal X-ray diffraction analysis reveals that the distortion of the Pb octahedra is influenced by the stereochemistry of the cations and their interactions with the perovskite layers. Solid-state 1H and 207Pb NMR spectroscopy analysis further confirms this trend, whereby different 1H and 207Pb chemical shifts are observed for the pPDA and mPDA spacer cations, indicating different hydrogen-bonding interactions and octahedral distortions. Owing to the octahedral distortion, 2D (mPDA)PbBr4 compounds exhibit broader white-light emission than 2D (pPDA)PbBr4. Density functional theory calculations suggest that (pPDA)PbBr4 and (mPDA)PbBr4 are direct-band-gap semiconductors, and they exhibit larger electronic band gaps and effective masses than the Ruddlesden-Popper-phase (BA)2PbBr4. Among the films of these compounds, 2D (mPDA)PbBr4 shows the best stability, which is attributed to stronger hydrogen-bonding interactions in the material.
引用
收藏
页码:9685 / 9698
页数:14
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