Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells
Abstract
The presence of unreacted lead iodide in organic-inorganic lead halide perovskite solar cells is widely correlated with an increase in power conversion efficiency. We investigate the mechanism for this increase by identifying the role of surfaces and interfaces present between methylammonium lead iodide perovskite films and excess lead iodide. We show how type I and II band alignments arising under different conditions result in either passivation of surface defects or hole injection. Through first-principles simulations of solid-solid interfaces, we find that lead iodide captures holes from methylammonium lead iodide and modulates the formation of defects in the perovskite, affecting recombination. Using surface-sensitive optical spectroscopy techniques, such as transient reflectance and time-resolved photoluminescence, we show how excess lead iodide affects the diffusion and surface recombination velocity of charge carriers in methylammonium lead iodide films. Our coupled experimental and theoretical results elucidate the role of excess lead iodide in perovskite solar cells.
- Authors:
-
[1];
[2];
[2];
[2];
[3]
- Univ. of Chicago, IL (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1871660
- Report Number(s):
- NREL/JA-5900-82034
Journal ID: ISSN 2380-8195; MainId:82807;UUID:535d0032-3707-4722-9480-0b55bae79136;MainAdminID:64626
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Energy Letters
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; metal halide perovskite; transient spectroscopy
Citation Formats
Ahmad, Zeeshan, Scheidt, Rebecca A., Hautzinger, Matthew P., Zhu, Kai, Beard, Matthew C., and Galli, Giulia. Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells. United States: N. p., 2022.
Web. doi:10.1021/acsenergylett.2c00850.
Ahmad, Zeeshan, Scheidt, Rebecca A., Hautzinger, Matthew P., Zhu, Kai, Beard, Matthew C., & Galli, Giulia. Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells. United States. https://doi.org/10.1021/acsenergylett.2c00850
Ahmad, Zeeshan, Scheidt, Rebecca A., Hautzinger, Matthew P., Zhu, Kai, Beard, Matthew C., and Galli, Giulia. Tue .
"Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells". United States. https://doi.org/10.1021/acsenergylett.2c00850. https://www.osti.gov/servlets/purl/1871660.
@article{osti_1871660,
title = {Understanding the Effect of Lead Iodide Excess on the Performance of Methylammonium Lead Iodide Perovskite Solar Cells},
author = {Ahmad, Zeeshan and Scheidt, Rebecca A. and Hautzinger, Matthew P. and Zhu, Kai and Beard, Matthew C. and Galli, Giulia},
abstractNote = {The presence of unreacted lead iodide in organic-inorganic lead halide perovskite solar cells is widely correlated with an increase in power conversion efficiency. We investigate the mechanism for this increase by identifying the role of surfaces and interfaces present between methylammonium lead iodide perovskite films and excess lead iodide. We show how type I and II band alignments arising under different conditions result in either passivation of surface defects or hole injection. Through first-principles simulations of solid-solid interfaces, we find that lead iodide captures holes from methylammonium lead iodide and modulates the formation of defects in the perovskite, affecting recombination. Using surface-sensitive optical spectroscopy techniques, such as transient reflectance and time-resolved photoluminescence, we show how excess lead iodide affects the diffusion and surface recombination velocity of charge carriers in methylammonium lead iodide films. Our coupled experimental and theoretical results elucidate the role of excess lead iodide in perovskite solar cells.},
doi = {10.1021/acsenergylett.2c00850},
journal = {ACS Energy Letters},
number = 6,
volume = 7,
place = {United States},
year = {Tue May 10 00:00:00 EDT 2022},
month = {Tue May 10 00:00:00 EDT 2022}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Energy Level Tuning at the MAPbI 3 Perovskite/Contact Interface Using Chemical Treatment
journal, August 2019
- Meggiolaro, Daniele; Mosconi, Edoardo; Proppe, Andrew H.
- ACS Energy Letters, Vol. 4, Issue 9
Localized effect of PbI 2 excess in perovskite solar cells probed by high-resolution chemical–optoelectronic mapping
journal, January 2018
- Barbé, Jérémy; Newman, Michael; Lilliu, Samuele
- Journal of Materials Chemistry A, Vol. 6, Issue 45
Ionic transport in hybrid lead iodide perovskite solar cells
journal, June 2015
- Eames, Christopher; Frost, Jarvist M.; Barnes, Piers R. F.
- Nature Communications, Vol. 6, Issue 1
Individual Electron and Hole Mobilities in Lead-Halide Perovskites Revealed by Noncontact Methods
journal, November 2019
- Zhai, Yaxin; Wang, Kang; Zhang, Fei
- ACS Energy Letters, Vol. 5, Issue 1
Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts
journal, August 2019
- Yang, Shuang; Chen, Shangshang; Mosconi, Edoardo
- Science, Vol. 365, Issue 6452
Efficient perovskite solar cells via improved carrier management
journal, February 2021
- Yoo, Jason J.; Seo, Gabkyung; Chua, Matthew R.
- Nature, Vol. 590, Issue 7847
Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells
journal, March 2020
- Ni, Zhenyi; Bao, Chunxiong; Liu, Ye
- Science, Vol. 367, Issue 6484
Observation of spatially resolved Rashba states on the surface of CH 3 NH 3 PbBr 3 single crystals
journal, September 2021
- Huang, Zhengjie; Vardeny, Shai R.; Wang, Tonghui
- Applied Physics Reviews, Vol. 8, Issue 3
Light-induced annihilation of Frenkel defects in organo-lead halide perovskites
journal, January 2016
- Mosconi, Edoardo; Meggiolaro, Daniele; Snaith, Henry J.
- Energy & Environmental Science, Vol. 9, Issue 10
Understanding the physical properties of hybrid perovskites for photovoltaic applications
journal, July 2017
- Huang, Jinsong; Yuan, Yongbo; Shao, Yuchuan
- Nature Reviews Materials, Vol. 2, Issue 7
Band offsets and dielectric properties of the amorphous Si 3 N 4 /Si(100) interface: A first-principles study
journal, June 2013
- Anh Pham, T.; Li, Tianshu; Nguyen, Huy-Viet
- Applied Physics Letters, Vol. 102, Issue 24
Geometric and electronic structures of interfaces
journal, March 2001
- Yamasaki, Takahiro; Kaneta, Chioko; Uchiyama, Toshihiro
- Physical Review B, Vol. 63, Issue 11
Charge-Carrier Mobilities in Metal Halide Perovskites: Fundamental Mechanisms and Limits
journal, June 2017
- Herz, Laura M.
- ACS Energy Letters, Vol. 2, Issue 7
Critical Assessment of the Use of Excess Lead Iodide in Lead Halide Perovskite Solar Cells
journal, July 2020
- Roose, Bart; Dey, Krishanu; Chiang, Yu-Hsien
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 16
Formation of a passivating CH 3 NH 3 PbI 3 /PbI 2 interface during moderate heating of CH 3 NH 3 PbI 3 layers
journal, October 2013
- Supasai, T.; Rujisamphan, N.; Ullrich, K.
- Applied Physics Letters, Vol. 103, Issue 18
Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films
journal, January 2017
- Yang, Ye; Yang, Mengjin; Moore, David T.
- Nature Energy, Vol. 2, Issue 2
The emergence of perovskite solar cells
journal, July 2014
- Green, Martin A.; Ho-Baillie, Anita; Snaith, Henry J.
- Nature Photonics, Vol. 8, Issue 7, p. 506-514
Rashba–Dresselhaus Effect in Inorganic/Organic Lead Iodide Perovskite Interfaces
journal, May 2018
- Myung, Chang Woo; Javaid, Saqib; Kim, Kwang S.
- ACS Energy Letters, Vol. 3, Issue 6
Atomic-scale microstructure of metal halide perovskite
journal, October 2020
- Rothmann, Mathias Uller; Kim, Judy S.; Borchert, Juliane
- Science, Vol. 370, Issue 6516
Iodine chemistry determines the defect tolerance of lead-halide perovskites
journal, January 2018
- Meggiolaro, Daniele; Motti, Silvia G.; Mosconi, Edoardo
- Energy & Environmental Science, Vol. 11, Issue 3
Qresp, a tool for curating, discovering and exploring reproducible scientific papers
journal, January 2019
- Govoni, Marco; Munakami, Milson; Tanikanti, Aditya
- Scientific Data, Vol. 6, Issue 1
Unreacted PbI 2 as a Double-Edged Sword for Enhancing the Performance of Perovskite Solar Cells
journal, August 2016
- Jacobsson, T. Jesper; Correa-Baena, Juan-Pablo; Halvani Anaraki, Elham
- Journal of the American Chemical Society, Vol. 138, Issue 32
Modulating crystal grain size and optoelectronic properties of perovskite films for solar cells by reaction temperature
journal, January 2016
- Ren, Xiaodong; Yang, Zhou; Yang, Dong
- Nanoscale, Vol. 8, Issue 6
Defect migration in methylammonium lead iodide and its role in perovskite solar cell operation
journal, January 2015
- Azpiroz, Jon M.; Mosconi, Edoardo; Bisquert, Juan
- Energy & Environmental Science, Vol. 8, Issue 7
Iodine interstitials as a cause of nonradiative recombination in hybrid perovskites
journal, April 2020
- Zhang, Xie; Turiansky, Mark E.; Shen, Jimmy-Xuan
- Physical Review B, Vol. 101, Issue 14
The role of PbI 2 in CH 3 NH 3 PbI 3 perovskite stability, solar cell parameters and device degradation
journal, January 2018
- Gujar, Tanaji P.; Unger, Thomas; Schönleber, Andreas
- Physical Chemistry Chemical Physics, Vol. 20, Issue 1
Photovoltaic Performance of Perovskite Solar Cells with Different Grain Sizes
journal, December 2015
- Kim, Hyung Do; Ohkita, Hideo; Benten, Hiroaki
- Advanced Materials, Vol. 28, Issue 5
Formation of Surface Defects Dominates Ion Migration in Lead-Halide Perovskites
journal, February 2019
- Meggiolaro, Daniele; Mosconi, Edoardo; De Angelis, Filippo
- ACS Energy Letters, Vol. 4, Issue 3
Density Functional Calculations of Native Defects in CH 3 NH 3 PbI 3 : Effects of Spin–Orbit Coupling and Self-Interaction Error
journal, April 2015
- Du, Mao-Hua
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 8
Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013
- Stranks, S. D.; Eperon, G. E.; Grancini, G.
- Science, Vol. 342, Issue 6156, p. 341-344
Controllable Self-Induced Passivation of Hybrid Lead Iodide Perovskites toward High Performance Solar Cells
journal, June 2014
- Chen, Qi; Zhou, Huanping; Song, Tze-Bin
- Nano Letters, Vol. 14, Issue 7
Adverse Effects of Excess Residual PbI 2 on Photovoltaic Performance, Charge Separation, and Trap-State Properties in Mesoporous Structured Perovskite Solar Cells
journal, February 2017
- Wang, Hao-Yi; Hao, Ming-Yang; Han, Jun
- Chemistry - A European Journal, Vol. 23, Issue 16
Ultrafast probes at the interfaces of solar energy conversion materials
journal, January 2019
- Chen, Xihan; Wang, Kang; Beard, Matthew C.
- Physical Chemistry Chemical Physics, Vol. 21, Issue 30
Observation of lower defect density brought by excess PbI 2 in CH 3 NH 3 PbI 3 solar cells
journal, August 2019
- Jiang, Minlin; Wu, Yuxia; Zhou, Yi
- AIP Advances, Vol. 9, Issue 8
Stability of Organic Cations in Solution-Processed CH 3 NH 3 PbI 3 Perovskites: Formation of Modified Surface Layers
journal, September 2015
- Calloni, A.; Abate, A.; Bussetti, G.
- The Journal of Physical Chemistry C, Vol. 119, Issue 37
Interfaces in metal halide perovskites probed by solid-state NMR spectroscopy
journal, January 2021
- Dahlman, Clayton J.; Kubicki, Dominik J.; Reddy, G. N. Manjunatha
- Journal of Materials Chemistry A, Vol. 9, Issue 35
Unraveling the Passivation Process of PbI 2 to Enhance the Efficiency of Planar Perovskite Solar Cells
journal, August 2018
- Shi, Biao; Yao, Xin; Hou, Fuhua
- The Journal of Physical Chemistry C, Vol. 122, Issue 37
Chemically diverse and multifunctional hybrid organic–inorganic perovskites
journal, February 2017
- Li, Wei; Wang, Zheming; Deschler, Felix
- Nature Reviews Materials, Vol. 2, Issue 3
High efficiency methylammonium lead triiodide perovskite solar cells: the relevance of non-stoichiometric precursors
journal, January 2015
- Roldán-Carmona, C.; Gratia, P.; Zimmermann, I.
- Energy & Environmental Science, Vol. 8, Issue 12
Impact of Excess Lead Iodide on the Recombination Kinetics in Metal Halide Perovskites
journal, May 2019
- Merdasa, Aboma; Kiligaridis, Alexander; Rehermann, Carolin
- ACS Energy Letters, Vol. 4, Issue 6
Is Excess PbI 2 Beneficial for Perovskite Solar Cell Performance?
journal, January 2016
- Liu, Fangzhou; Dong, Qi; Wong, Man Kwong
- Advanced Energy Materials, Vol. 6, Issue 7
Termination Dependence of Tetragonal CH 3 NH 3 PbI 3 Surfaces for Perovskite Solar Cells
journal, August 2014
- Haruyama, Jun; Sodeyama, Keitaro; Han, Liyuan
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 16
Controlling competing photochemical reactions stabilizes perovskite solar cells
journal, May 2019
- Motti, Silvia G.; Meggiolaro, Daniele; Barker, Alex J.
- Nature Photonics, Vol. 13, Issue 8
Ultrafast ion migration in hybrid perovskite polycrystalline thin films under light and suppression in single crystals
journal, January 2016
- Xing, Jie; Wang, Qi; Dong, Qingfeng
- Physical Chemistry Chemical Physics, Vol. 18, Issue 44