Critical Role of Water in Defect Aggregation and Chemical Degradation of Perovskite Solar Cells
File(s)
Accepted version
OA Location
Author(s)
Kye, Yun-Hyok
Yu, Chol-Jun
Jong, Un-Gi
Chen, Yue
Walsh, Aron
Type
Journal Article
Abstract
The chemical stability of methylammonium lead iodide (MAPbI3) under humid conditions remains the primary challenge facing halide perovskite solar cells. We investigate defect processes in the water-intercalated iodide perovskite (MAPbI3_H2O) and monohydrated phase (MAPbI3·H2O) within a first-principles thermodynamic framework. We consider the formation energies of isolated and aggregated vacancy defects with different charge states under I-rich and I-poor conditions. It is found that a PbI2 (partial Schottky) vacancy complex can be formed readily, while the MAI vacancy complex is difficult to form in the hydrous compounds. Vacancies in the hydrous phases create deep charge transition levels, indicating the degradation of the lead halide perovskite upon exposure to moisture. Electronic structure analysis supports a mechanism of water-mediated vacancy pair formation.
Date Issued
2018-05-03
Date Acceptance
2018-04-12
Citation
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2018, 9 (9), pp.2196-2201
ISSN
1948-7185
Publisher
American Chemical Society
Start Page
2196
End Page
2201
Journal / Book Title
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume
9
Issue
9
Copyright Statement
© 2018 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry Letters, after peer review and technical editing by the publisher. To access the final edited and published work see https://dx.doi.org/10.1021/acs.jpclett.8b00406
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000431724400014&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Technology
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Physics, Atomic, Molecular & Chemical
Chemistry
Science & Technology - Other Topics
Materials Science
Physics
METHYLAMMONIUM LEAD IODIDE
HALIDE PEROVSKITES
PHOTOVOLTAIC EFFICIENCY
CH3NH3PBI3 PEROVSKITE
ELECTRONIC-STRUCTURE
AB-INITIO
CH(3)NH(3)PBL(3)
STABILITY
TRANSPORT
STATE
Publication Status
Published
Date Publish Online
2018-04-12