Unravelling the Effects of Grain Boundary and Chemical Doping on Electron–Hole Recombination in CH 3 NH 3 PbI 3 Perovskite by Time-Domain Atomistic Simulation
Abstract
Advancing organohalide perovskite solar cells requires understanding of carrier dynamics. Electron–hole recombination is a particularly important process because it constitutes a major pathway of energy and current losses. Grain boundaries (GBs) are common in methylammonium lead iodine CH3NH3PbI3 (MAPbI3) perovskite polycrystalline films. First-principles calculations have suggested that GBs have little effect on the recombination; however, experiments defy this prediction. Using nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we show that GBs notably accelerate the electron–hole recombination in MAPbI3. First, GBs enhance the electron–phonon NA coupling by localizing and contributing to the electron and hole wave functions and by creating additional phonon modes that couple to the electronic degrees of freedom. Second, GBs decrease the MAPbI3 bandgap, reducing the number of vibrational quanta needed to accommodate the electronic energy loss. Third, the phonon-induced loss of electronic coherence remains largely unchanged and not accelerated, as one may expect from increased electron–phonon coupling. Further, replacing iodines by chlorines at GBs reduces the electron–hole recombination. By pushing the highest occupied molecular orbital (HOMO) density away from the boundary, chlorines restore the NA coupling close to the value observed in pristine MAPbI3. By introducing higher-frequency phonons and increasing fluctuation of the electronicmore »
- Authors:
-
- College of Chemistry, Key Laboratory of Theoretical & Computational Photochemistry of Ministry of Education, Beijing Normal University, Beijing 100875, P. R. China, School of Physics, Complex & Adaptive Systems Lab, University College Dublin, Dublin 4, Ireland
- Department of Chemical Engineering, University of Rochester, Rochester, New York 14627, United States
- Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
- Publication Date:
- Research Org.:
- Univ. of Southern California, Los Angeles, CA (United States). Dept. of Chemistry
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation of China; Science Foundation Ireland
- OSTI Identifier:
- 1241916
- Alternate Identifier(s):
- OSTI ID: 1437012
- Grant/Contract Number:
- SC0014429; 21573022; 1/SIRG/E2172
- Resource Type:
- Published Article
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Name: Journal of the American Chemical Society Journal Volume: 138 Journal Issue: 11; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Long, Run, Liu, Jin, and Prezhdo, Oleg V. Unravelling the Effects of Grain Boundary and Chemical Doping on Electron–Hole Recombination in CH 3 NH 3 PbI 3 Perovskite by Time-Domain Atomistic Simulation. United States: N. p., 2016.
Web. doi:10.1021/jacs.6b00645.
Long, Run, Liu, Jin, & Prezhdo, Oleg V. Unravelling the Effects of Grain Boundary and Chemical Doping on Electron–Hole Recombination in CH 3 NH 3 PbI 3 Perovskite by Time-Domain Atomistic Simulation. United States. https://doi.org/10.1021/jacs.6b00645
Long, Run, Liu, Jin, and Prezhdo, Oleg V. Thu .
"Unravelling the Effects of Grain Boundary and Chemical Doping on Electron–Hole Recombination in CH 3 NH 3 PbI 3 Perovskite by Time-Domain Atomistic Simulation". United States. https://doi.org/10.1021/jacs.6b00645.
@article{osti_1241916,
title = {Unravelling the Effects of Grain Boundary and Chemical Doping on Electron–Hole Recombination in CH 3 NH 3 PbI 3 Perovskite by Time-Domain Atomistic Simulation},
author = {Long, Run and Liu, Jin and Prezhdo, Oleg V.},
abstractNote = {Advancing organohalide perovskite solar cells requires understanding of carrier dynamics. Electron–hole recombination is a particularly important process because it constitutes a major pathway of energy and current losses. Grain boundaries (GBs) are common in methylammonium lead iodine CH3NH3PbI3 (MAPbI3) perovskite polycrystalline films. First-principles calculations have suggested that GBs have little effect on the recombination; however, experiments defy this prediction. Using nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we show that GBs notably accelerate the electron–hole recombination in MAPbI3. First, GBs enhance the electron–phonon NA coupling by localizing and contributing to the electron and hole wave functions and by creating additional phonon modes that couple to the electronic degrees of freedom. Second, GBs decrease the MAPbI3 bandgap, reducing the number of vibrational quanta needed to accommodate the electronic energy loss. Third, the phonon-induced loss of electronic coherence remains largely unchanged and not accelerated, as one may expect from increased electron–phonon coupling. Further, replacing iodines by chlorines at GBs reduces the electron–hole recombination. By pushing the highest occupied molecular orbital (HOMO) density away from the boundary, chlorines restore the NA coupling close to the value observed in pristine MAPbI3. By introducing higher-frequency phonons and increasing fluctuation of the electronic gap, chlorines shorten electronic coherence. Both factors compete successfully with the reduced bandgap relative to pristine MAPbI3 and favor long excited-state lifetimes. The simulations show excellent agreement with experiment and characterize how GBs and chlorine dopants affect electron–hole recombination in perovskite solar cells. In conclusion, the simulations suggest a route to increased photon-to-electron conversion efficiencies through rational GB passivation.},
doi = {10.1021/jacs.6b00645},
journal = {Journal of the American Chemical Society},
number = 11,
volume = 138,
place = {United States},
year = {Thu Mar 10 00:00:00 EST 2016},
month = {Thu Mar 10 00:00:00 EST 2016}
}
https://doi.org/10.1021/jacs.6b00645
Web of Science
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