Layer Distortion Engineering for Spontaneous Charge Separation in Two-Dimensional Perovskites

被引：2

作者：

Zhao, Chunyi ^{[1
,2
]}

Bao, Jingwen ^{[3
,4
,5
]}

Gao, Yan ^{[6
,7
]}

Yan, Xianchang ^{[3
,4
]}

Sun, Fengke ^{[3
,4
]}

Cheng, Hui ^{[3
,4
,5
]}

Chen, Longwen ^{[1
,2
]}

Lv, Haifeng ^{[6
,7
]}

Yao, Guanxin ^{[1
,2
]}

Zhang, Xianyi ^{[1
,2
]}

Tian, Wenming ^{[3
,4
]}

Jin, Shengye ^{[3
,4
]}

Wu, Xiaojun ^{[6
,7
]}

Sun, Qi ^{[3
,4
]}

Lu, Zhou ^{[1
,2
]}

机构：

[1] Anhui Normal Univ, Minist Educ, Key Lab Funct Mol Solids, Anhui Prov Key Lab Control & Applicat Optoelect In, Wuhu 241002, Peoples R China

[2] Anhui Normal Univ, Anhui Engn Res Ctr Carbon Neutral, Wuhu 241002, Peoples R China

[3] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China

[4] Chinese Acad Sci, Dalian Inst Chem Phys, Dynam Res Ctr Energy & Environm Mat, Dalian 116023, Peoples R China

[5] Dalian Univ Technol, Sch Phys, Sch Microelect, Key Lab Mat Modificat Laser Ion & Electron Beams,M, Dalian 116024, Peoples R China

[6] Univ Sci & Technol China, Sch Chem & Mat Sci, Key Lab Precis & Intelligent Chem, CAS Key Lab Mat Energy Convers, Hefei 230026, Anhui, Peoples R China

[7] Univ Sci & Technol China, Collaborat Innovat Ctr Chem Energy Mat iChEM, Hefei 230026, Anhui, Peoples R China

来源：

ACS ENERGY LETTERS | 2024年 / 9卷 / 10期

基金：

中国国家自然科学基金;

关键词：

EXCITON BINDING-ENERGY; BROAD-BAND EMISSION; TRANSIENT-ABSORPTION; DYNAMICS; GERMANIUM; ORIGINS; FILM;

D O I：

10.1021/acsenergylett.4c02099

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：

Charge separation in highly confined type-I two-dimensional (2D) perovskites with a single inorganic layer (n = 1) remains challenging due to their excessive exciton binding energy. Herein, we engineer the layer distortion within Ruddlesden-Popper (RP) type perovskites (n = 1) by tailoring the sizes of the cycloalkylamine ligands. The perovskite layers are more distorted and corrugated to accommodate the highly compact yet rigid cyclopropylammonium and cyclobutylammonium, facilitating the formation of Pb-Pb and I-I ionic dimers as self-localizing sites for charge carriers. Consequently, spontaneous electron-hole separation as well as a long-lived (>1 mu s) intrinsic quantum confined Stark effect (QCSE) is achieved using the thresholdless optical pump and without applying any external electric field, yielding an unprecedent amount of the photoinduced bandgap energy lowering. This work opens up new possibilities of efficient charge separation in type-I 2D quantum wells for the photovoltaic and nonlinear optical modulation applications.

引用

页码：4994 / 5001

页数：8

共 46 条

[1] A deconvoluted PL approach to probe the charge carrier dynamics of the grain interior and grain boundary of a perovskite film for perovskite solar cell applications [J].