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The Mechanism of Slow Hot-Hole Cooling in Lead-Iodide Perovskite: First-Principles Calculation on Carrier Lifetime from Electron–Phonon Interaction
Abstract
We report on an analysis of hot-carrier lifetimes from electron-phonon interaction in lead iodide perovskites using first-principles calculations. Our calculations show that the holes in CsPbI3 have very long lifetimes in the valence band region situated 0.6 eV below the top of the valence band. On the other hand, no long lifetime is predicted in PbI3(-). These different results reflect the different electronic density of states (DOSs) in the valence bands, that is, a small DOS for the former structure while a sharp DOS peak for the latter structure. We propose a reduction of the relaxation paths in the small valence DOS as being the origin of the slow hot-hole cooling. Analyzing the generalized Eliashberg functions, we predict that different perovskite A-site cations do not have an impact on the carrier decay mechanism. The similarity between the DOS structures of CsPbI3 and CH3NH3PbI3 enables us to extend the description of the decay mechanism of fully inorganic CsPbI3 to its organic-inorganic counterpart, CH3NH3PbI3.
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Cites
Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells
Jeon, N. J., Noh, J. H., Kim, Y. C., Yang, W. S., Ryu, S., & Seok, S. I. (2014) · Nature Materials · doi:10.1038/nmat4014 · Cited by 6,723
Cited by
Electron–phonon coupling in hybrid lead halide perovskites
Wright, A. D., Verdi, C., Milot, R. L., Eperon, G. E., Pérez-Osorio, M. A., Snaith, H. J., Giustino, F., Johnston, M. B., & Herz, L. M. (2016) · Nature Communications · doi:10.1038/ncomms11755 · Cited by 1,374
Charge-Carrier Dynamics in Organic-Inorganic Metal Halide Perovskites
Herz, L. M. (2016) · Annual Review of Physical Chemistry · doi:10.1146/annurev-physchem-040215-112222 · Cited by 819
Zhu, X.-Y., & Podzorov, V. (2015) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.5b02462 · Cited by 608
Rashba Spin–Orbit Coupling Enhanced Carrier Lifetime in CH3NH3PbI3
Zheng, F., Tan, L. Z., Liu, S., & Rappe, A. M. (2015) · Nano Letters · doi:10.1021/acs.nanolett.5b01854 · Cited by 507
Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites
Yang, J., Wen, X., Xia, H., Sheng, R., Ma, Q., Kim, J., Tapping, P., Harada, T., Kee, T. W., Huang, F., et al. (2017) · Nature Communications · doi:10.1038/ncomms14120 · Cited by 503
Metadata
- Authors
- Kawai, H., Giorgi, G., Marini, A., & Yamashita, K.
- Venue
- Nano Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-04-01
- Volume
- 15
- Issue
- 5
- Pages
- 3103-3108
- ISSN
- 1530-6984 (ISSN-L)
- 1530-6992
- OpenAlex
- W2326081621
- Cited by
- 180
- References
- 1
- FWCI
- 11.07
- Type
- journal article
- Language
- en
- Open access
- closed
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- Kawai, H., Giorgi, G., Marini, A., & Yamashita, K. (2015). The Mechanism of Slow Hot-Hole Cooling in Lead-Iodide Perovskite: First-Principles Calculation on Carrier Lifetime from Electron–Phonon Interaction. Nano Letters. https://doi.org/10.1021/acs.nanolett.5b00109
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