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Title: Metal/Ion Interactions Induced p–i–n Junction in Methylammonium Lead Triiodide Perovskite Single Crystals

Abstract

Hybrid perovskites, as emerging multifunctional semiconductors, have demonstrated dual electronic/ionic conduction properties. Here, we report a metal/ion interaction induced p-i-n junction across slightly n-type doped MAPbI3 single crystals with Au/MAPbI3/Ag configuration based on interface dependent Seebeck effect, Hall effect and time-of-flight secondary ion mass spectrometry analysis. The organic cations (MA+) interact with Au atoms, forming positively charged coordination complexes at Au/MAPbI3 interface, whereas iodine anions (I) can react with Ag contacts, leading to interfacial ionic polarization. Such metal/ion interactions establish a p-doped region near the Au/MAPbI3 interface due to the formation of MA+ vacancies, and an n-doped region near the Ag/MAPbI3 interface due to formation of I vacancies, consequently forming a p-i-n junction across the crystal in Au/MAPbI3/Ag configuration. Therefore, the metal/ion interaction plays a role in determining the surface electronic structure and semiconducting properties of hybrid perovskites.

Authors:
 [1];  [1];  [2];  [2];  [1]; ORCiD logo [3]; ORCiD logo [3];  [3];  [2];  [1]; ORCiD logo [1]
  1. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Inst. for Functional Imaging of Materials
  3. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); National Science Foundation of China
OSTI Identifier:
1422483
Grant/Contract Number:  
AC05-00OR22725; FA 9550-15-1-0064; 21161160445
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 48; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wu, Ting, Mukherjee, Rupam, Ovchinnikova, Olga S., Collins, Liam, Ahmadi, Mahshid, Lu, Wei, Kang, Nam-Goo, Mays, Jimmy W., Jesse, Stephen, Mandrus, David, and Hu, Bin. Metal/Ion Interactions Induced p–i–n Junction in Methylammonium Lead Triiodide Perovskite Single Crystals. United States: N. p., 2017. Web. https://doi.org/10.1021/jacs.7b10416.
Wu, Ting, Mukherjee, Rupam, Ovchinnikova, Olga S., Collins, Liam, Ahmadi, Mahshid, Lu, Wei, Kang, Nam-Goo, Mays, Jimmy W., Jesse, Stephen, Mandrus, David, & Hu, Bin. Metal/Ion Interactions Induced p–i–n Junction in Methylammonium Lead Triiodide Perovskite Single Crystals. United States. https://doi.org/10.1021/jacs.7b10416
Wu, Ting, Mukherjee, Rupam, Ovchinnikova, Olga S., Collins, Liam, Ahmadi, Mahshid, Lu, Wei, Kang, Nam-Goo, Mays, Jimmy W., Jesse, Stephen, Mandrus, David, and Hu, Bin. Fri . "Metal/Ion Interactions Induced p–i–n Junction in Methylammonium Lead Triiodide Perovskite Single Crystals". United States. https://doi.org/10.1021/jacs.7b10416. https://www.osti.gov/servlets/purl/1422483.
@article{osti_1422483,
title = {Metal/Ion Interactions Induced p–i–n Junction in Methylammonium Lead Triiodide Perovskite Single Crystals},
author = {Wu, Ting and Mukherjee, Rupam and Ovchinnikova, Olga S. and Collins, Liam and Ahmadi, Mahshid and Lu, Wei and Kang, Nam-Goo and Mays, Jimmy W. and Jesse, Stephen and Mandrus, David and Hu, Bin},
abstractNote = {Hybrid perovskites, as emerging multifunctional semiconductors, have demonstrated dual electronic/ionic conduction properties. Here, we report a metal/ion interaction induced p-i-n junction across slightly n-type doped MAPbI3 single crystals with Au/MAPbI3/Ag configuration based on interface dependent Seebeck effect, Hall effect and time-of-flight secondary ion mass spectrometry analysis. The organic cations (MA+) interact with Au atoms, forming positively charged coordination complexes at Au/MAPbI3 interface, whereas iodine anions (I–) can react with Ag contacts, leading to interfacial ionic polarization. Such metal/ion interactions establish a p-doped region near the Au/MAPbI3 interface due to the formation of MA+ vacancies, and an n-doped region near the Ag/MAPbI3 interface due to formation of I– vacancies, consequently forming a p-i-n junction across the crystal in Au/MAPbI3/Ag configuration. Therefore, the metal/ion interaction plays a role in determining the surface electronic structure and semiconducting properties of hybrid perovskites.},
doi = {10.1021/jacs.7b10416},
journal = {Journal of the American Chemical Society},
number = 48,
volume = 139,
place = {United States},
year = {2017},
month = {11}
}

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