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Formation of Surface Defects Dominates Ion Migration in Lead-Halide Perovskites
Abstract
We propose a new model of defect formation and ion migration at the surfaces/grain boundaries of lead-halide perovskites, based on ab initio calculations. Inspired by the spread of experimentally measured activation energies for ion migration in similar lead-iodide perovskites, we define an effective defect formation energy weighed upon surface and bulk contributions. We thus link the large variation in measured activation energies for ion migration to the different defect formation energies of polycrystalline thin films with different grains size. Defect formation is facilitated at surfaces; thus, smaller grains exhibit an averagely lower activation energy to ion migration than larger grains. We also account for the increased ion migration observed under light. Overall, our findings point at surface passivation as a major direction to stabilize lead-halide perovskites against formation of defects, limiting in turn the the associated decomposition reactions.
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Stranks, S. D., Eperon, G. E., Grancini, G., Menelaou, C., Alcocer, M. J. P., Leijtens, T., Herz, L. M., Petrozza, A., & Snaith, H. J. (2013) · Science · doi:10.1126/science.1243982 · Cited by 10,413
Impact of microstructure on local carrier lifetime in perovskite solar cells
de Quilettes, D. W., Vorpahl, S. M., Stranks, S. D., Nagaoka, H., Eperon, G. E., Ziffer, M. E., Snaith, H. J., & Ginger, D. S. (2015) · Science · doi:10.1126/science.aaa5333 · Cited by 2,198
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Defect engineering of two-dimensional materials for advanced energy conversion and storage
Liu, F., & Fan, Z. (2023) · Chemical Society Reviews · doi:10.1039/d2cs00931e · Cited by 417
Futscher, M. H., Lee, J. M., McGovern, L., Muscarella, L. A., Wang, T., Haider, M. I., Fakharuddin, A., Schmidt-Mende, L., & Ehrler, B. (2019) · Materials Horizons · doi:10.1039/c9mh00445a · Cited by 409
Zhou, Y., Herz, L. M., Jen, A. K.-Y., & Saliba, M. (2022) · Nature Energy · doi:10.1038/s41560-022-01096-5 · Cited by 281
Low-temperature carbon-based electrodes in perovskite solar cells
Bogachuk, D., Zouhair, S., Wojciechowski, K., Yang, B., Babu, V., Wagner, L., Xu, B., Lim, J., Mastroianni, S., Pettersson, H., et al. (2020) · Energy & Environmental Science · doi:10.1039/d0ee02175j · Cited by 268
Metadata
- Authors
- Meggiolaro, D., Mosconi, E., & De Angelis, F.
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-02-20
- Volume
- 4
- Issue
- 3
- Pages
- 779-785
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W2916785621
- Cited by
- 386
- References
- 2
- FWCI
- 14.28
- Type
- journal article
- Language
- en
- Open access
- closed
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- Meggiolaro, D., Mosconi, E., & De Angelis, F. (2019). Formation of Surface Defects Dominates Ion Migration in Lead-Halide Perovskites. ACS Energy Letters. https://doi.org/10.1021/acsenergylett.9b00247
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