Role of Lead Vacancies for Optoelectronic Properties of Lead-Halide Perovskites
Abstract
Methylammonium lead iodide perovskite materials have been shown to be efficient in photovoltaic devices. The current fabrication process has not been perfected, leaving defects such as site vacancies, which can trap charge and have a detrimental effect on photogenerated charge carriers. Here focus is placed on the effect a Pb site vacancy has on the charge-carrier dynamics following photoexcitation. The electronic structure of materials with vacancies is often found in open-shell configurations with unpaired electrons in the conduction/valence bands To accurately describe unpaired electrons, spin-polarized and noncollinear spin calculations are performed on both neutral and charged vacancy systems. This work presents spin-polarized and noncollinear spin ground-state electronic structures and nonradiative rates of charge-carrier relaxation and introduces an extension to a novel procedure to compute photoluminescence spectra for open-shell models. This study describes nonadiabatic dynamics of MAPbI3 models within a Redfield formalism focusing on the role of a Pb vacancy defect on electronic relaxation processes. Results show the vacancy of the Pb ion introducing a new energy state within the unblemished material band gap region. Finally, this additional unoccupied state is expected to increase the nonradiative relaxation lifetime of the excited electron, allowing for a longer lifetime of the charge carriermore »
- Authors:
-
- Univ. of South Dakota, Vermillion, SD (United States). Dept. of Chemistry
- L.N. Gumilyov Eurasian National Univ., Astana (Kazakhstan); National Univ. of Science and Technology, Moscow (Russia)
- Univ. of South Dakota, Vermillion, SD (United States). Dept. of Chemistry; North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1480500
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 10; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Vogel, Dayton J., Inerbaev, Talgat M., and Kilin, Dmitri S. Role of Lead Vacancies for Optoelectronic Properties of Lead-Halide Perovskites. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b05375.
Vogel, Dayton J., Inerbaev, Talgat M., & Kilin, Dmitri S. Role of Lead Vacancies for Optoelectronic Properties of Lead-Halide Perovskites. United States. https://doi.org/10.1021/acs.jpcc.7b05375
Vogel, Dayton J., Inerbaev, Talgat M., and Kilin, Dmitri S. Mon .
"Role of Lead Vacancies for Optoelectronic Properties of Lead-Halide Perovskites". United States. https://doi.org/10.1021/acs.jpcc.7b05375. https://www.osti.gov/servlets/purl/1480500.
@article{osti_1480500,
title = {Role of Lead Vacancies for Optoelectronic Properties of Lead-Halide Perovskites},
author = {Vogel, Dayton J. and Inerbaev, Talgat M. and Kilin, Dmitri S.},
abstractNote = {Methylammonium lead iodide perovskite materials have been shown to be efficient in photovoltaic devices. The current fabrication process has not been perfected, leaving defects such as site vacancies, which can trap charge and have a detrimental effect on photogenerated charge carriers. Here focus is placed on the effect a Pb site vacancy has on the charge-carrier dynamics following photoexcitation. The electronic structure of materials with vacancies is often found in open-shell configurations with unpaired electrons in the conduction/valence bands To accurately describe unpaired electrons, spin-polarized and noncollinear spin calculations are performed on both neutral and charged vacancy systems. This work presents spin-polarized and noncollinear spin ground-state electronic structures and nonradiative rates of charge-carrier relaxation and introduces an extension to a novel procedure to compute photoluminescence spectra for open-shell models. This study describes nonadiabatic dynamics of MAPbI3 models within a Redfield formalism focusing on the role of a Pb vacancy defect on electronic relaxation processes. Results show the vacancy of the Pb ion introducing a new energy state within the unblemished material band gap region. Finally, this additional unoccupied state is expected to increase the nonradiative relaxation lifetime of the excited electron, allowing for a longer lifetime of the charge carrier and increased opportunity for secondary relaxation mechanisms or collection to take place.},
doi = {10.1021/acs.jpcc.7b05375},
journal = {Journal of Physical Chemistry. C},
number = 10,
volume = 122,
place = {United States},
year = {Mon Dec 18 00:00:00 EST 2017},
month = {Mon Dec 18 00:00:00 EST 2017}
}
Web of Science
Figures / Tables:
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