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

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

doi:10.1038/ncomms14120

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

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

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

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Abstract

The hot-phonon bottleneck effect in lead-halide perovskites (APbX₃) 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 FAPbI₃. 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.

Original language	English
Article number	14120
Number of pages	9
Journal	Nature Communications
Volume	8
DOIs	https://doi.org/10.1038/ncomms14120
Publication status	Published - 20 Jan 2017
Externally published	Yes

Bibliographical note

Copyright the Author(s) 2017. Version archived for private and non-commercial use with the permission of the author/s and according to publisher conditions. For further rights please contact the publisher.

Keywords

CARRIER SOLAR-CELLS
QUANTUM-WELLS
EFFICIENCY
FILMS
1ST-PRINCIPLES
CH3NH3PBI3
GENERATION
EMISSION
LIFETIME
SPECTRUM

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10.1038/ncomms14120Licence: CC BY

Publisher version (open access)Final published version, 915 KBLicence: CC BY

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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, 8, Article 14120. https://doi.org/10.1038/ncomms14120

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abstract = "The hot-phonon bottleneck effect in lead-halide perovskites (APbX3) 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 FAPbI3. 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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AU - Xia, Hongze

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AU - Ma, Qingshan

AU - Kim, Jincheol

AU - Tapping, Patrick

AU - Harada, Takaaki

AU - Kee, Tak W.

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AU - Cheng, Yi-Bing

AU - Green, Martin

AU - Ho-Baillie, Anita

AU - Huang, Shujuan

AU - Shrestha, Santosh

AU - Patterson, Robert

AU - Conibeer, Gavin

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PY - 2017/1/20

Y1 - 2017/1/20

N2 - The hot-phonon bottleneck effect in lead-halide perovskites (APbX3) 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 FAPbI3. 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.

AB - The hot-phonon bottleneck effect in lead-halide perovskites (APbX3) 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 FAPbI3. 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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Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites

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