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Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells
Open accessAbstract
Abstract Halide perovskites show unusual thermalization kinetics for above-bandgap photoexcitation. We explain this as a consequence of excess energy being deposited into discrete large polaron states. The crossover between low-fluence and high-fluence “phonon bottleneck” cooling is due to a Mott transition where the polarons overlap (n ≥ 1018 cm–3) and the phonon subpopulations are shared. We calculate the initial rate of cooling (thermalization) from the scattering time in the Fröhlich polaron model to be 78 meV ps–1 for CH3NH3PbI3. This rapid initial thermalization involves heat transfer into optical phonon modes coupled by a polar dielectric interaction. Further cooling to equilibrium over hundreds of picoseconds is limited by the ultralow thermal conductivity of the perovskite lattice.
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Cites
Price, M. B., Butkus, J., Jellicoe, T. C., Sadhanala, A., Briane, A., Halpert, J. E., Broch, K., Hodgkiss, J. M., Friend, R. H., & Deschler, F. (2015) · Nature Communications · doi:10.1038/ncomms9420 · Cited by 704
Cited by
Fu, Y., Zhu, H., Chen, J., Hautzinger, M. P., Zhu, X.-Y., & Jin, S. (2019) · Nature Reviews Materials · doi:10.1038/s41578-019-0080-9 · Cited by 934
Zheng, Q., Chu, W., Zhao, C., Zhang, L., Guo, H., Wang, Y., Jiang, X., & Zhao, J. (2019) · WIREs Computational Molecular Science · doi:10.1002/wcms.1411 · Cited by 452
Performance-limiting nanoscale trap clusters at grain junctions in halide perovskites
Doherty, T. A. S., Winchester, A. J., Macpherson, S., Johnstone, D. N., Pareek, V., Tennyson, E. M., Kosar, S., Kosasih, F. U., Anaya, M., Abdi-Jalebi, M., et al. (2020) · Nature · doi:10.1038/s41586-020-2184-1 · Cited by 369
Self-citationDefect Activity in Lead Halide Perovskites
Motti, S. G., Meggiolaro, D., Martani, S., Sorrentino, R., Barker, A. J., De Angelis, F., & Petrozza, A. (2019) · Advanced Materials · doi:10.1002/adma.201901183 · Cited by 331
Metadata
- Authors
- Frost, J. M., Whalley, L. D., & Walsh, A.
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-10-27
- Volume
- 2
- Issue
- 12
- Pages
- 2647-2652
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W2745311780
- Cited by
- 179
- References
- 1
- FWCI
- 7.94
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Frost, J. M., Whalley, L. D., & Walsh, A. (2017). Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells. ACS Energy Letters. https://doi.org/10.1021/acsenergylett.7b00862
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Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.
