Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties
Abstract
In this paper, the nanoscale through-film and lateral photo-response and conductivity of large-grained methylammonium lead iodide (MAPbI3) thin films are studied. In perovskite solar cells (PSC), these films result in efficiencies >17%. The grain boundaries (GBs) show high resistance at the top surface of the film, and act as an impediment to photocurrent collection. However, lower resistance pathways between grains exist below the top surface of the film, indicating that there exists a depth-dependent resistance of GBs (RGB(z)). Furthermore, lateral conductivity measurements indicate that RGB(z) exhibits GB-to-GB heterogeneity. These results indicate that increased photocurrent collection along GBs is not a prerequisite for high-efficiency PSCs. Rather, better control of depth-dependent GB electrical properties, and an improvement in the homogeneity of the GB-to-GB electrical properties, must be managed to enable further improvements in PSC efficiency. Finally, these results refute the implicit assumption seen in the literature that the electrical properties of GBs, as measured at the top surface of the perovskite film, necessarily reflect the electrical properties of GBs within the thickness of the film.
- Authors:
-
- National Inst. of Standards and Technology (NIST), Boulder, CO (United States). Material Measurement Lab., Applied Chemicals and Materials Division
- National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center
- National Inst. of Standards and Technology (NIST), Boulder, CO (United States). Physical Measurement Lab., Applied Physics Division
- National Renewable Energy Lab. (NREL), Golden, CO (United States). National Center for Photovoltaics
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1339245
- Report Number(s):
- NREL/JA-5900-67690
Journal ID: ISSN 1754-5692; EESNBY
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Energy & Environmental Science
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 1754-5692
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; nanoscale; methylammonium lead iodide thin films
Citation Formats
MacDonald, Gordon A., Yang, Mengjin, Berweger, Samuel, Killgore, Jason P., Kabos, Pavel, Berry, Joseph J., Zhu, Kai, and DelRio, Frank W. Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties. United States: N. p., 2016.
Web. doi:10.1039/C6EE01889K.
MacDonald, Gordon A., Yang, Mengjin, Berweger, Samuel, Killgore, Jason P., Kabos, Pavel, Berry, Joseph J., Zhu, Kai, & DelRio, Frank W. Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties. United States. https://doi.org/10.1039/C6EE01889K
MacDonald, Gordon A., Yang, Mengjin, Berweger, Samuel, Killgore, Jason P., Kabos, Pavel, Berry, Joseph J., Zhu, Kai, and DelRio, Frank W. Fri .
"Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties". United States. https://doi.org/10.1039/C6EE01889K. https://www.osti.gov/servlets/purl/1339245.
@article{osti_1339245,
title = {Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties},
author = {MacDonald, Gordon A. and Yang, Mengjin and Berweger, Samuel and Killgore, Jason P. and Kabos, Pavel and Berry, Joseph J. and Zhu, Kai and DelRio, Frank W.},
abstractNote = {In this paper, the nanoscale through-film and lateral photo-response and conductivity of large-grained methylammonium lead iodide (MAPbI3) thin films are studied. In perovskite solar cells (PSC), these films result in efficiencies >17%. The grain boundaries (GBs) show high resistance at the top surface of the film, and act as an impediment to photocurrent collection. However, lower resistance pathways between grains exist below the top surface of the film, indicating that there exists a depth-dependent resistance of GBs (RGB(z)). Furthermore, lateral conductivity measurements indicate that RGB(z) exhibits GB-to-GB heterogeneity. These results indicate that increased photocurrent collection along GBs is not a prerequisite for high-efficiency PSCs. Rather, better control of depth-dependent GB electrical properties, and an improvement in the homogeneity of the GB-to-GB electrical properties, must be managed to enable further improvements in PSC efficiency. Finally, these results refute the implicit assumption seen in the literature that the electrical properties of GBs, as measured at the top surface of the perovskite film, necessarily reflect the electrical properties of GBs within the thickness of the film.},
doi = {10.1039/C6EE01889K},
journal = {Energy & Environmental Science},
number = 12,
volume = 9,
place = {United States},
year = {Fri Sep 23 00:00:00 EDT 2016},
month = {Fri Sep 23 00:00:00 EDT 2016}
}
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Works referenced in this record:
Reversible Hydration of CH 3 NH 3 PbI 3 in Films, Single Crystals, and Solar Cells
journal, April 2015
- Leguy, Aurélien M. A.; Hu, Yinghong; Campoy-Quiles, Mariano
- Chemistry of Materials, Vol. 27, Issue 9
Employing Lead Thiocyanate Additive to Reduce the Hysteresis and Boost the Fill Factor of Planar Perovskite Solar Cells
journal, May 2016
- Ke, Weijun; Xiao, Chuanxiao; Wang, Changlei
- Advanced Materials, Vol. 28, Issue 26
Benefit of Grain Boundaries in Organic–Inorganic Halide Planar Perovskite Solar Cells
journal, February 2015
- Yun, Jae S.; Ho-Baillie, Anita; Huang, Shujuan
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 5
Grain-Boundary-Enhanced Carrier Collection in CdTe Solar Cells
journal, April 2014
- Li, Chen; Wu, Yelong; Poplawsky, Jonathan
- Physical Review Letters, Vol. 112, Issue 15
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
Grain-Size-Limited Mobility in Methylammonium Lead Iodide Perovskite Thin Films
journal, August 2016
- Reid, Obadiah G.; Yang, Mengjin; Kopidakis, Nikos
- ACS Energy Letters, Vol. 1, Issue 3
Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009
- Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo
- Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051
Square-Centimeter Solution-Processed Planar CH 3 NH 3 PbI 3 Perovskite Solar Cells with Efficiency Exceeding 15%
journal, September 2015
- Yang, Mengjin; Zhou, Yuanyuan; Zeng, Yining
- Advanced Materials, Vol. 27, Issue 41
Impact of microstructure on local carrier lifetime in perovskite solar cells
journal, April 2015
- de Quilettes, D. W.; Vorpahl, S. M.; Stranks, S. D.
- Science, Vol. 348, Issue 6235
Grain boundary dominated ion migration in polycrystalline organic–inorganic halide perovskite films
journal, January 2016
- Shao, Yuchuan; Fang, Yanjun; Li, Tao
- Energy & Environmental Science, Vol. 9, Issue 5
Reduction of grain boundary recombination in polycrystalline silicon solar cells
journal, April 1977
- DiStefano, T. H.; Cuomo, J. J.
- Applied Physics Letters, Vol. 30, Issue 7
Origin and elimination of photocurrent hysteresis by fullerene passivation in CH3NH3PbI3 planar heterojunction solar cells
journal, December 2014
- Shao, Yuchuan; Xiao, Zhengguo; Bi, Cheng
- Nature Communications, Vol. 5, Issue 1
Electrical testing of gold nanostructures by conducting atomic force microscopy
journal, January 2000
- Bietsch, Alexander; Schneider, M. Alexander; Welland, Mark E.
- Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 18, Issue 3
Coarsening of one-step deposited organolead triiodide perovskite films via Ostwald ripening for high efficiency planar-heterojunction solar cells
journal, January 2016
- Zhu, Weidong; Bao, Chunxiong; Wang, Yangrunqian
- Dalton Transactions, Vol. 45, Issue 18
Theoretical and experimental investigations of nano-Schottky contacts
journal, July 2016
- Rezeq, Moh'd; Eledlebi, Khouloud; Ismail, Mohammed
- Journal of Applied Physics, Vol. 120, Issue 4
Solution Chemistry Engineering toward High-Efficiency Perovskite Solar Cells
journal, November 2014
- Zhao, Yixin; Zhu, Kai
- The Journal of Physical Chemistry Letters, Vol. 5, Issue 23
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
Contact Mechanics
journal, October 1986
- Johnson, K. L.; Keer, L. M.
- Journal of Tribology, Vol. 108, Issue 4
Heterogeneous Charge Carrier Dynamics in Organic–Inorganic Hybrid Materials: Nanoscale Lateral and Depth-Dependent Variation of Recombination Rates in Methylammonium Lead Halide Perovskite Thin Films
journal, June 2015
- Bischak, Connor G.; Sanehira, Erin M.; Precht, Jake T.
- Nano Letters, Vol. 15, Issue 7
Perovskite-based solar cells: impact of morphology and device architecture on device performance
journal, January 2015
- Salim, Teddy; Sun, Shuangyong; Abe, Yuichiro
- Journal of Materials Chemistry A, Vol. 3, Issue 17
Perovskite Solar Cells: From Materials to Devices
journal, October 2014
- Jung, Hyun Suk; Park, Nam-Gyu
- Small, Vol. 11, Issue 1
Grain-boundary recombination in Cu(In,Ga)Se2 solar cells
journal, December 2005
- Gloeckler, Markus; Sites, James R.; Metzger, Wyatt K.
- Journal of Applied Physics, Vol. 98, Issue 11
Humidity-Induced Grain Boundaries in MAPbI 3 Perovskite Films
journal, March 2016
- Li, Dan; Bretschneider, Simon A.; Bergmann, Victor W.
- The Journal of Physical Chemistry C, Vol. 120, Issue 12
Study on the stability of CH 3 NH 3 PbI 3 films and the effect of post-modification by aluminum oxide in all-solid-state hybrid solar cells
journal, January 2014
- Niu, Guangda; Li, Wenzhe; Meng, Fanqi
- J. Mater. Chem. A, Vol. 2, Issue 3
Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells
journal, April 2014
- Frost, Jarvist M.; Butler, Keith T.; Brivio, Federico
- Nano Letters, Vol. 14, Issue 5
The light and shade of perovskite solar cells
journal, August 2014
- Grätzel, Michael
- Nature Materials, Vol. 13, Issue 9
Microscopic Investigation of Grain Boundaries in Organolead Halide Perovskite Solar Cells
journal, December 2015
- Li, Jiang-Jun; Ma, Jing-Yuan; Ge, Qian-Qing
- ACS Applied Materials & Interfaces, Vol. 7, Issue 51
Transformation of the Excited State and Photovoltaic Efficiency of CH 3 NH 3 PbI 3 Perovskite upon Controlled Exposure to Humidified Air
journal, January 2015
- Christians, Jeffrey A.; Miranda Herrera, Pierre A.; Kamat, Prashant V.
- Journal of the American Chemical Society, Vol. 137, Issue 4
Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9%
journal, August 2012
- Kim, Hui-Seon; Lee, Chang-Ryul; Im, Jeong-Hyeok
- Scientific Reports, Vol. 2, Issue 1
Works referencing / citing this record:
Defect Engineering toward Highly Efficient and Stable Perovskite Solar Cells
journal, July 2018
- Li, Bowei; Ferguson, Victoria; Silva, S. Ravi P.
- Advanced Materials Interfaces, Vol. 5, Issue 22
Interface Engineering in Tin Perovskite Solar Cells
journal, October 2019
- Gao, Weiyin; Li, Peizhou; Chen, Jinbo
- Advanced Materials Interfaces, Vol. 6, Issue 24
Edge Effect on the Population of Free Carriers and Excitons in Single‐Crystal CH 3 NH 3 PbBr 3 Perovskite Nanomaterials
journal, May 2019
- Zhang, Zhen‐Yu; Yu, Kuai; Wang, Guo‐Ping
- Advanced Electronic Materials, Vol. 5, Issue 7
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
Oriented Grains with Preferred Low-Angle Grain Boundaries in Halide Perovskite Films by Pressure-Induced Crystallization
journal, December 2017
- Kim, Wanjung; Jung, Myung Sun; Lee, Seonhee
- Advanced Energy Materials, Vol. 8, Issue 10
Capturing the Sun: A Review of the Challenges and Perspectives of Perovskite Solar Cells
journal, January 2018
- Petrus, Michiel L.; Schlipf, Johannes; Li, Cheng
- Advanced Energy Materials, Vol. 8, Issue 2
Imaging Metal Halide Perovskites Material and Properties at the Nanoscale
journal, December 2019
- Howard, John M.; Lahoti, Richa; Leite, Marina S.
- Advanced Energy Materials
Perowskit-Solarzellen: atomare Ebene, Schichtqualität und Leistungsfähigkeit der Zellen
journal, February 2018
- Saliba, Michael; Correa-Baena, Juan-Pablo; Grätzel, Michael
- Angewandte Chemie, Vol. 130, Issue 10
Perovskite Solar Cells: From the Atomic Level to Film Quality and Device Performance
journal, February 2018
- Saliba, Michael; Correa-Baena, Juan-Pablo; Grätzel, Michael
- Angewandte Chemie International Edition, Vol. 57, Issue 10
Imaging material functionality through three-dimensional nanoscale tracking of energy flow
journal, October 2019
- Delor, Milan; Weaver, Hannah L.; Yu, QinQin
- Nature Materials, Vol. 19, Issue 1
Identifying the charge generation dynamics in Cs + -based triple cation mixed perovskite solar cells
journal, January 2017
- Salado, Manuel; Kokal, Ramesh K.; Calio, Laura
- Physical Chemistry Chemical Physics, Vol. 19, Issue 34
Approaching the Shockley–Queisser limit for fill factors in lead–tin mixed perovskite photovoltaics
journal, January 2020
- Jayawardena, K. D. G. I.; Bandara, R. M. I.; Monti, M.
- Journal of Materials Chemistry A, Vol. 8, Issue 2
Tin( iv ) dopant removal through anti-solvent engineering enabling tin based perovskite solar cells with high charge carrier mobilities
journal, January 2019
- Bandara, R. M. I.; Jayawardena, K. D. G. I.; Adeyemo, S. O.
- Journal of Materials Chemistry C, Vol. 7, Issue 27
Tin(iv) dopant removal through anti-solvent engineering enabling tin based perovskite solar cells with high charge carrier mobilities
text, January 2019
- Bandara, Rmi; Jayawardena, Kdgi; Adeyemo, Stephanie
- Apollo - University of Cambridge Repository
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