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Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites

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Yang, Jianfeng, Wen, Xiaoming, Xia, Hongze, Sheng, Rui, Ma, Qingshan, Kim, Jincheol, Tapping, Patrick, Harada, Takaaki, Kee, Tak W., Huang, Fuzhi, Cheng, Yi-Bing, Green, Martin, Ho-Baillie, Anita, Huang, Shujuan, Shrestha, Santosh, Patterson, Robert, Conibeer, Gavin·2017·Nature Communications

Abstract

The hot-phonon bottleneck effect in lead-halide perovskites (APbX 3) prolongs the cooling period of hot charge carriers, an effect that could be used in the next-generation photovoltaics devices. Using ultrafast optical characterization and first-principle calculations, four kinds of lead-halide perovskites (A=FA+/MA+/Cs+, X=I−/Br−) are compared in this study to reveal the carrier-phonon dynamics within. Here we show a stronger phonon bottleneck effect in hybrid perovskites than in their inorganic counterparts. Compared with the caesium-based system, a 10 times slower carrier-phonon relaxation rate is observed in FAPbI 3. The up-conversion of low-energy phonons is proposed to be responsible for the bottleneck effect. The presence of organic cations introduces overlapping phonon branches and facilitates the up-transition of low-energy modes. The blocking of phonon propagation associated with an ultralow thermal conductivity of the material also increases the overall up-conversion efficiency. This result also suggests a new and general method for achieving long-lived hot carriers in materials.

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Metadata

Authors
Yang, J., Wen, X., Xia, H., Sheng, R., Ma, Q., Kim, J., Tapping, P., Harada, T., Kee, T. W., Huang, F., Cheng, Y.-B., Green, M., Ho-Baillie, A., Huang, S., Shrestha, S., Patterson, R., & Conibeer, G.
Venue
Nature Communications
Published
2017-01-20
Volume
8
Issue
1
Pages
14120-14120
ISSN
2041-1723 (ISSN-L)
OpenAlex
W2577497532
Cited by
503
References
47
FWCI
21.37
Type
journal article
Language
en
Open access
gold

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CoChat. (2026). Citation check: Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites. https://app.cochat.ai/papers/10.1038/ncomms14120
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Yang, J., Wen, X., Xia, H., Sheng, R., Ma, Q., Kim, J., Tapping, P., Harada, T., Kee, T. W., Huang, F., Cheng, Y.-B., Green, M., Ho-Baillie, A., Huang, S., Shrestha, S., Patterson, R., & Conibeer, G. (2017). Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites. Nature Communications. https://doi.org/10.1038/ncomms14120

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