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

被引：24

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

来源：

CHEMISTRY OF MATERIALS | 2022年 / 34卷 / 21期

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

页码：9685 / 9698

页数：14

共 62 条

[1] Dion-Jacobson Phase 2D Layered Perovskites for Solar Cells with Ultrahigh Stability (vol 3, pg 794, 2019) [J].