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Local Polar Fluctuations in Lead Halide Perovskite Crystals
Open accessAbstract
Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low-frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in the cubic phase of both hybrid (CH_{3}NH_{3}PbBr_{3}) and all-inorganic (CsPbBr_{3}) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations indicate that head-to-head Cs motion coupled to Br face expansion, occurring on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr_{3}.
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Cites
Real-Time Observation of Organic Cation Reorientation in Methylammonium Lead Iodide Perovskites
Bakulin, A. A., Selig, O., Bakker, H. J., Rezus, Y. L. A., Müller, C., Glaser, T., Lovrincic, R., Sun, Z., Chen, Z., Walsh, A., et al. (2015) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.5b01555 · Cited by 372
Cited by
Synthetic Approaches for Halide Perovskite Thin Films
Dunlap-Shohl, W. A., Zhou, Y., Padture, N. P., & Mitzi, D. B. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00318 · Cited by 631
Structural Diversity in White-Light-Emitting Hybrid Lead Bromide Perovskites
Mao, L., Guo, P., Kepenekian, M., Hadar, I., Katan, C., Even, J., Schaller, R. D., Stoumpos, C. C., & Kanatzidis, M. G. (2018) · Journal of the American Chemical Society · doi:10.1021/jacs.8b08691 · Cited by 508
Self-citationThouin, F., Valverde-Chávez, D. A., Quarti, C., Cortecchia, D., Bargigia, I., Beljonne, D., Petrozza, A., Silva, C., & Srimath Kandada, A. R. (2019) · Nature Materials · doi:10.1038/s41563-018-0262-7 · Cited by 384
Structural and thermodynamic limits of layer thickness in 2D halide perovskites
Soe, C. M. M., Nagabhushana, G. P., Shivaramaiah, R., Tsai, H., Nie, W., Blancon, J.-C., Melkonyan, F., Cao, D. H., Traoré, B., Pedesseau, L., et al. (2019) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1811006115 · Cited by 363
Self-citationXie, H., Hao, S., Bao, J., Slade, T. J., Snyder, G. J., Wolverton, C., & Kanatzidis, M. G. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.0c03427 · Cited by 298
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Metadata
- Authors
- Yaffe, O., Guo, Y., Tan, L. Z., Egger, D. A., Hull, T., Stoumpos, C. C., Zheng, F., Heinz, T. F., Kronik, L., Kanatzidis, M. G., Owen, J. S., Rappe, A. M., Pimenta, M. A., & Brus, L. E.
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2017-03-28
- Volume
- 118
- Issue
- 13
- Pages
- 136001-136001
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W2533641981
- Cited by
- 694
- References
- 1
- FWCI
- 31.55
- Type
- journal article
- Language
- en
- Open access
- green
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- Yaffe, O., Guo, Y., Tan, L. Z., Egger, D. A., Hull, T., Stoumpos, C. C., Zheng, F., Heinz, T. F., Kronik, L., Kanatzidis, M. G., Owen, J. S., Rappe, A. M., Pimenta, M. A., & Brus, L. E. (2017). Local Polar Fluctuations in Lead Halide Perovskite Crystals. Physical Review Letters. https://doi.org/10.1103/physrevlett.118.136001
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