Dangling Octahedra Enable Edge States in 2D Lead Halide Perovskites

Qin, Yan1,2,3; Li, Zhi-Gang1; Gao, Fei-Fei1; Chen, Haisheng4,5; Li, Xiang6; Xu, Bin7,8; Li, Qian7,8; Jiang, Xingxing9; Li, Wei1; Wu, Xiang6; Quan, Zewei7,8; Ye, Lei10; Zhang, Yang4,5; Lin, Zheshuai9; Pedesseau, Laurent11; Even, Jacky11; Lu, Peixiang2,3; Bu, Xian-He1

2022-06-01

10.1002/adma.202201666

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

The structural reconstruction at the crystal layer edges of 2D lead halide perovskites (LHPs) leads to unique edge states (ES), which are manifested by prolonged carrier lifetime and reduced emission energy. These special ES can effectively enhance the optoelectronic performance of devices, but their intrinsic origin and working mechanism remain elusive. Here it is demonstrated that the ES of a family of 2D Ruddlesden-Popper LHPs [BA(2)CsPb(2)Br(7), BA(2)MAPb(2)Br(7), and BA(2)MA(2)Pb(3)Br(10) (BA = butylammonium; MA = methylammonium)] arise from the rotational symmetry elevation of the PbBr6 octahedra dangling at the crystal layer edges. These dangling octahedra give rise to localized electronic states that enable an effective transport of electrons from the interior to layer edges, and the population of electrons in both the interior states and the ES can be manipulated via controlling the external fields. Moreover, the abundant phonons, activated by the dangling octahedra, can interact with electrons to facilitate radiative recombination, counterintuitive to the suppressive role commonly observed in conventional semiconductors. This work unveils the intrinsic atomistic and electronic origins of ES in 2D LHPs, which can stimulate the exploration of ES-based exotic optoelectronic properties and the corresponding design of high-performance devices for these emergent low-dimensional semiconductors.

2D lead halide perovskites dangling octahedra edge states electron-phonon interactions local symmetry

SCI ; EI

英语

NI论文

其他

National Natural Science Foundation of China[21975132,21991143,11874230] ; Fundamental Research Funds for the Central Universities[63196006] ; Natural Science Foundation of Tianjin[18JCYBJC41500] ; 111 project from China[B18030] ; European Union's Horizon 2020 research and innovation programme[899141] ; GENCI[2021-A0100911434]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000811806900001

WILEY-V C H VERLAG GMBH

20222512237202

Carrier lifetime ; Crystal symmetry ; Electronic states ; Electrons ; Lead compounds ; Perovskite ; Phonons

Minerals:482.2 ; Electricity: Basic Concepts and Phenomena:701.1 ; Crystal Lattice:933.1.1 ; Electronic Structure of Solids:933.3

MATERIALS SCIENCE

Web of Science

1.Nankai Univ, Sch Mat Sci & Engn, Tianjin Key Lab Met & Mol Mat Chem, Tianjin 300350, Peoples R China
2.Huazhong Univ Sci & Technol, Sch Phys, Wuhan 430074, Peoples R China
3.Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Peoples R China
4.Nankai Univ, Inst Modern Opt, Tianjin 300350, Peoples R China
5.Nankai Univ, Tianjin Key Lab MicroScale Opt Informat Sci & Tec, Tianjin 300350, Peoples R China
6.China Univ Geosci, State Key Lab Geol Proc & Mineral Resources, Wuhan 430074, Peoples R China
7.Southern Univ Sci & Technol SUSTech, Dept Chem, Acad Adv Interdisciplinary Studies, Shenzhen 518055, Peoples R China
8.Southern Univ Sci & Technol SUSTech, Shenzhen Engn Res Ctr Frontier Mat Synth High Pre, Shenzhen 518055, Peoples R China
9.Chinese Acad Sci, Tech Inst Phys & Chem, Beijing 100190, Peoples R China
10.Huazhong Univ Sci & Technol, Sch Opt & Elect Informat, Wuhan 430074, Peoples R China
11.Univ Rennes, INSA Rennes, CNRS, Inst FOTON,UMR 6082, F-35000 Rennes, France

Qin, Yan,Li, Zhi-Gang,Gao, Fei-Fei,et al. Dangling Octahedra Enable Edge States in 2D Lead Halide Perovskites[J]. ADVANCED MATERIALS,2022,34.

Qin, Yan.,Li, Zhi-Gang.,Gao, Fei-Fei.,Chen, Haisheng.,Li, Xiang.,...&Bu, Xian-He.(2022).Dangling Octahedra Enable Edge States in 2D Lead Halide Perovskites.ADVANCED MATERIALS,34.

Qin, Yan,et al."Dangling Octahedra Enable Edge States in 2D Lead Halide Perovskites".ADVANCED MATERIALS 34(2022).