{"title":"Layer Distortion Engineering for Spontaneous Charge Separation in Two-Dimensional Perovskites","authors":"Chunyi Zhao, Jingwen Bao, Yan Gao, Xianchang Yan, Fengke Sun, Hui Cheng, Longwen Chen, Haifeng Lv, Guanxin Yao, Xianyi Zhang, Wenming Tian, Shengye Jin, Xiaojun Wu, Qi Sun, Zhou Lu","doi":"10.1021/acsenergylett.4c02099","DOIUrl":null,"url":null,"abstract":"Charge separation in highly confined type-I two-dimensional (2D) perovskites with a single inorganic layer (<i>n</i> = 1) remains challenging due to their excessive exciton binding energy. Herein, we engineer the layer distortion within Ruddlesden–Popper (RP) type perovskites (<i>n</i> = 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 μs) 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.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":19.3000,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Energy Letters ","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsenergylett.4c02099","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
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 μs) 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.
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍:
ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format.
ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology.
The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.