Defect Energetics in Pseudo-Cubic Mixed Halide Lead Perovskites from First-Principles
Abstract
Owing to the increasing popularity of lead-based hybrid perovskites for photovoltaic (PV) applications, it is crucial to understand their defect energetics and its influence on their optoelectronic properties. In this work, we simulate various point defects in pseudocubic structures of mixed iodide-bromide and bromide-chloride methylammonium lead perovskites with the general formula MAPbI3-yBry or MAPbBr3-yCly (where y is between 0 and 3), and use first-principles based density functional theory computations to study their relative formation energies and charge transition levels. We identify vacancy defects and Pb on MA antisite defect as the lowest energy native defects in each perovskite. Here, we observe that while the low energy defects in all MAPbI3-yBry systems only create shallow transition levels, the Br or Cl vacancy defects in the Cl-containing pervoskites have low energy and form deep levels which become deeper for higher Cl content. We examine the structures and density of states of pure and defect-containing perovskite systems to obtain an understanding of the nature of defect levels. Further, we study extrinsic substitution by different elements at the Pb site in MAPbBr3, MAPbCl3, and the 50-50 mixed halide perovskite, MAPbBr1.5Cl1.5, and identify some transition metals that create lower energy defects than the dominant intrinsicmore »
- Authors:
-
[1];
[1];
[1]
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Imperial College, London (United Kingdom)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1762154
- Grant/Contract Number:
- AC02-06CH11357; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 31; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; impurities; energy; defects; electrical conductivity; perovskites
Citation Formats
Mannodi-Kanakkithodi, Arun, Park, Ji-Sang, Martinson, Alex F., and Chan, Maria Y. Defect Energetics in Pseudo-Cubic Mixed Halide Lead Perovskites from First-Principles. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcc.0c02486.
Mannodi-Kanakkithodi, Arun, Park, Ji-Sang, Martinson, Alex F., & Chan, Maria Y. Defect Energetics in Pseudo-Cubic Mixed Halide Lead Perovskites from First-Principles. United States. https://doi.org/10.1021/acs.jpcc.0c02486
Mannodi-Kanakkithodi, Arun, Park, Ji-Sang, Martinson, Alex F., and Chan, Maria Y. Mon .
"Defect Energetics in Pseudo-Cubic Mixed Halide Lead Perovskites from First-Principles". United States. https://doi.org/10.1021/acs.jpcc.0c02486. https://www.osti.gov/servlets/purl/1762154.
@article{osti_1762154,
title = {Defect Energetics in Pseudo-Cubic Mixed Halide Lead Perovskites from First-Principles},
author = {Mannodi-Kanakkithodi, Arun and Park, Ji-Sang and Martinson, Alex F. and Chan, Maria Y.},
abstractNote = {Owing to the increasing popularity of lead-based hybrid perovskites for photovoltaic (PV) applications, it is crucial to understand their defect energetics and its influence on their optoelectronic properties. In this work, we simulate various point defects in pseudocubic structures of mixed iodide-bromide and bromide-chloride methylammonium lead perovskites with the general formula MAPbI3-yBry or MAPbBr3-yCly (where y is between 0 and 3), and use first-principles based density functional theory computations to study their relative formation energies and charge transition levels. We identify vacancy defects and Pb on MA antisite defect as the lowest energy native defects in each perovskite. Here, we observe that while the low energy defects in all MAPbI3-yBry systems only create shallow transition levels, the Br or Cl vacancy defects in the Cl-containing pervoskites have low energy and form deep levels which become deeper for higher Cl content. We examine the structures and density of states of pure and defect-containing perovskite systems to obtain an understanding of the nature of defect levels. Further, we study extrinsic substitution by different elements at the Pb site in MAPbBr3, MAPbCl3, and the 50-50 mixed halide perovskite, MAPbBr1.5Cl1.5, and identify some transition metals that create lower energy defects than the dominant intrinsic defects and also create midgap charge transition levels.},
doi = {10.1021/acs.jpcc.0c02486},
journal = {Journal of Physical Chemistry. C},
number = 31,
volume = 124,
place = {United States},
year = {Mon Jul 06 00:00:00 EDT 2020},
month = {Mon Jul 06 00:00:00 EDT 2020}
}
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