Photo-induced halide redistribution in organic–inorganic perovskite films
Abstract
Organic-inorganic perovskites such as CH3NH3PbI3 are promising materials for a variety of optoelectronic applications, with certified power conversion efficiencies in solar cells already exceeding 21%. Nevertheless, state-of-the-art films still contain performance-limiting non-radiative recombination sites and exhibit a range of complex dynamic phenomena under illumination that remain poorly understood. Here we use a unique combination of confocal photoluminescence (PL) microscopy and chemical imaging to correlate the local changes in photophysics with composition in CH3NH3PbI3 films under illumination. We demonstrate that the photo-induced 'brightening' of the perovskite PL can be attributed to an order-of-magnitude reduction in trap state density. By imaging the same regions with time-of-flight secondary-ion-mass spectrometry, we correlate this photobrightening with a net migration of iodine. In conclusion, our work provides visual evidence for photo-induced halide migration in triiodide perovskites and reveals the complex interplay between charge carrier populations, electronic traps and mobile halides that collectively impact optoelectronic performance.
- Authors:
-
- Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
- Univ. of Lincoln, Lincoln (United Kingdom). School of Chemistry
- Univ. of Oxford, Oxford (United Kingdom). Dept. of Physics; Mathematical Inst., OCCAM
- Univ. of Washington, Seattle, WA (United States). Dept. of Bioengineering
- Univ. of Oxford, Oxford (United Kingdom). Dept. of Physics
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Laboratory of Electronics
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Laboratory of Electronics; Cavendish Laboratory, Cambridge (United Kingdom)
- Publication Date:
- Research Org.:
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States).
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1282930
- Grant/Contract Number:
- SC0013957; SC0001088
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; solar-cells; anomalous hysteresis; lead-iodide; single-crystals; thin-films; photoluminescence; CH3NH3PbI3; electron; diffusion; recombination
Citation Formats
deQuilettes, Dane W., Zhang, Wei, Burlakov, Victor M., Graham, Daniel J., Leijtens, Tomas, Osherov, Anna, Bulovic, Vladimir, Snaith, Henry J., Ginger, David S., and Stranks, Samuel D. Photo-induced halide redistribution in organic–inorganic perovskite films. United States: N. p., 2016.
Web. doi:10.1038/ncomms11683.
deQuilettes, Dane W., Zhang, Wei, Burlakov, Victor M., Graham, Daniel J., Leijtens, Tomas, Osherov, Anna, Bulovic, Vladimir, Snaith, Henry J., Ginger, David S., & Stranks, Samuel D. Photo-induced halide redistribution in organic–inorganic perovskite films. United States. https://doi.org/10.1038/ncomms11683
deQuilettes, Dane W., Zhang, Wei, Burlakov, Victor M., Graham, Daniel J., Leijtens, Tomas, Osherov, Anna, Bulovic, Vladimir, Snaith, Henry J., Ginger, David S., and Stranks, Samuel D. Tue .
"Photo-induced halide redistribution in organic–inorganic perovskite films". United States. https://doi.org/10.1038/ncomms11683. https://www.osti.gov/servlets/purl/1282930.
@article{osti_1282930,
title = {Photo-induced halide redistribution in organic–inorganic perovskite films},
author = {deQuilettes, Dane W. and Zhang, Wei and Burlakov, Victor M. and Graham, Daniel J. and Leijtens, Tomas and Osherov, Anna and Bulovic, Vladimir and Snaith, Henry J. and Ginger, David S. and Stranks, Samuel D.},
abstractNote = {Organic-inorganic perovskites such as CH3NH3PbI3 are promising materials for a variety of optoelectronic applications, with certified power conversion efficiencies in solar cells already exceeding 21%. Nevertheless, state-of-the-art films still contain performance-limiting non-radiative recombination sites and exhibit a range of complex dynamic phenomena under illumination that remain poorly understood. Here we use a unique combination of confocal photoluminescence (PL) microscopy and chemical imaging to correlate the local changes in photophysics with composition in CH3NH3PbI3 films under illumination. We demonstrate that the photo-induced 'brightening' of the perovskite PL can be attributed to an order-of-magnitude reduction in trap state density. By imaging the same regions with time-of-flight secondary-ion-mass spectrometry, we correlate this photobrightening with a net migration of iodine. In conclusion, our work provides visual evidence for photo-induced halide migration in triiodide perovskites and reveals the complex interplay between charge carrier populations, electronic traps and mobile halides that collectively impact optoelectronic performance.},
doi = {10.1038/ncomms11683},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Tue May 24 00:00:00 EDT 2016},
month = {Tue May 24 00:00:00 EDT 2016}
}
Web of Science
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- Li, Bowei; Ferguson, Victoria; Silva, S. Ravi P.
- Advanced Materials Interfaces, Vol. 5, Issue 22
Capturing the Sun: A Review of the Challenges and Perspectives of Perovskite Solar Cells
journal, June 2017
- Petrus, Michiel L.; Schlipf, Johannes; Li, Cheng
- Advanced Energy Materials, Vol. 7, Issue 16
Impact of Structural Dynamics on the Optical Properties of Methylammonium Lead Iodide Perovskites
journal, June 2017
- Panzer, Fabian; Li, Cheng; Meier, Tobias
- Advanced Energy Materials, Vol. 7, Issue 16
Hybrid perovskite light emitting diodes under intense electrical excitation
journal, November 2018
- Kim, Hoyeon; Zhao, Lianfeng; Price, Jared S.
- Nature Communications, Vol. 9, Issue 1
High-performance and moisture-stable perovskite solar cells with a 2D modified layer via introducing a high dipole moment cation
journal, January 2019
- Xu, Huifen; Sun, Yuhai; Zheng, Haiying
- Journal of Materials Chemistry C, Vol. 7, Issue 48
How Methylammonium Cations and Chlorine Dopants Heal Defects in Lead Iodide Perovskites
journalarticle, January 2018
- Nan, G.; Zhang, X.; Abdi-Jalebi, M.
- Wiley
Elucidating the long-range charge carrier mobility in metal halide perovskite thin films
text, January 2018
- Lim, Jongchul; Hoerantner, Maximilian T.; Sakai, Nobuya
- arXiv
Long-Term Stabilization of Two-Dimensional Perovskites by Encapsulation with Hexagonal Boron Nitride
text, January 2020
- Seitz, Michael; Gant, Patricia; Castellanos-Gomez, Andres
- arXiv
High-Performance Planar Perovskite Solar Cells with Negligible Hysteresis Using 2,2,2-Trifluoroethanol-Incorporated SnO2
journal, June 2019
- Luan, Yigang; Yi, Xiaohui; Mao, Peng
- iScience, Vol. 16
Reversible Removal of Intermixed Shallow States by Light Soaking in Multication Mixed Halide Perovskite Films
journal, September 2019
- Guo, Dengyang; Andaji Garmaroudi, Zahra; Abdi-Jalebi, Mojtaba
- ACS Energy Letters, Vol. 4, Issue 10
Photoluminescence Blinking of Single-Crystal Methylammonium Lead Iodide Perovskite Nanorods Induced by Surface Traps
journal, July 2016
- Yuan, Haifeng; Debroye, Elke; Caliandro, Giorgio
- ACS Omega, Vol. 1, Issue 1
Statistics of the Auger Recombination of Electrons and Holes via Defect Levels in the Band Gap—Application to Lead-Halide Perovskites
journal, July 2018
- Staub, Florian; Rau, Uwe; Kirchartz, Thomas
- ACS Omega, Vol. 3, Issue 7
Defect-induced local variation of crystal phase transition temperature in metal-halide perovskites
journal, June 2017
- Dobrovolsky, Alexander; Merdasa, Aboma; Unger, Eva L.
- Nature Communications, Vol. 8, Issue 1
Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites
journal, August 2018
- Tan, Hairen; Che, Fanglin; Wei, Mingyang
- Nature Communications, Vol. 9, Issue 1
Transformation from crystalline precursor to perovskite in PbCl2-derived MAPbI3
journal, August 2018
- Stone, Kevin H.; Gold-Parker, Aryeh; Pool, Vanessa L.
- Nature Communications, Vol. 9, Issue 1
Hybrid perovskite light emitting diodes under intense electrical excitation
journal, November 2018
- Kim, Hoyeon; Zhao, Lianfeng; Price, Jared S.
- Nature Communications, Vol. 9, Issue 1
Unravelling the role of vacancies in lead halide perovskite through electrical switching of photoluminescence
journal, November 2018
- Li, Cheng; Guerrero, Antonio; Huettner, Sven
- Nature Communications, Vol. 9, Issue 1
Phase segregation due to ion migration in all-inorganic mixed-halide perovskite nanocrystals
journal, March 2019
- Zhang, Huichao; Fu, Xu; Tang, Ying
- Nature Communications, Vol. 10, Issue 1
Microscopic insight into non-radiative decay in perovskite semiconductors from temperature-dependent luminescence blinking
journal, April 2019
- Gerhard, Marina; Louis, Boris; Camacho, Rafael
- Nature Communications, Vol. 10, Issue 1
Graphite-protected CsPbBr3 perovskite photoanodes functionalised with water oxidation catalyst for oxygen evolution in water
journal, May 2019
- Poli, Isabella; Hintermair, Ulrich; Regue, Miriam
- Nature Communications, Vol. 10, Issue 1
Large lattice distortions and size-dependent bandgap modulation in epitaxial halide perovskite nanowires
journal, January 2020
- Oksenberg, Eitan; Merdasa, Aboma; Houben, Lothar
- Nature Communications, Vol. 11, Issue 1
Structural and Photophysical Properties of Methylammonium Lead Tribromide (MAPbBr3) Single Crystals
journal, October 2017
- Wang, Kai-Hung; Li, Liang-Chen; Shellaiah, Muthaiah
- Scientific Reports, Vol. 7, Issue 1
Electric Bias Induced Degradation in Organic-Inorganic Hybrid Perovskite Light-Emitting Diodes
journal, October 2018
- Xu, Bing; Wang, Weigao; Zhang, Xiaoli
- Scientific Reports, Vol. 8, Issue 1
Giant Zero-Drift Electronic Behaviors in Methylammonium Lead Halide Perovskite Diodes by Doping Iodine Ions
journal, September 2018
- Pang, Tiqiang; Jia, Renxu; Wang, Yucheng
- Materials, Vol. 11, Issue 9
Nanostructured Perovskite Solar Cells
journal, October 2019
- McDonald, Calum; Ni, Chengsheng; Maguire, Paul
- Nanomaterials, Vol. 9, Issue 10
Fractional Deviations in Precursor Stoichiometry Dictate the Properties, Performance and Stability of Perovskite Photovoltaic Devices
preprint, January 2019
- Fassl, Paul; Lami, Vincent; Bausch, Alexandra
- arXiv
Comparative studies of optoelectrical properties of prominent PV materials: Halide Perovskite, CdTe, and GaAs
text, January 2019
- Zhang, Fan; Castaneda, Jose F.; Chen, Shangshang
- arXiv
Visualizing buried local carrier diffusion in halide perovskite crystals via two-photon microscopy
preprint, January 2019
- Stavrakas, Camille; Delport, Géraud; Zhumekenov, Ayan A.
- arXiv
Nanoscale charge accumulation and its effect on carrier dynamics in tri-cation perovskite structures
preprint, January 2020
- Toth, David; Hailegnaw, Bekele; Richheimer, Filipe
- arXiv
Long-Term Stabilization of Two-Dimensional Perovskites by Encapsulation with Hexagonal Boron Nitride
text, January 2020
- Seitz, Michael; Gant, Patricia; Castellanos-Gomez, Andres
- arXiv
Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites
text, January 2017
- Wu, Xiaoxi; Tan, Liang Z.; Shen, Xiaozhe
- Columbia University