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 and Gavin Conibeer
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Jianfeng Yang: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Xiaoming Wen: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Hongze Xia: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Rui Sheng: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Qingshan Ma: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Jincheol Kim: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Patrick Tapping: The University of Adelaide
Takaaki Harada: The University of Adelaide
Tak W. Kee: The University of Adelaide
Fuzhi Huang: State Key Lab of Advanced Technologies for Materials Synthesis and Processing, Wuhan University of Technology
Yi-Bing Cheng: Monash University
Martin Green: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Anita Ho-Baillie: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Shujuan Huang: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Santosh Shrestha: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Robert Patterson: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales
Gavin Conibeer: Australian Centre for Advanced Photovoltaics, School of Photovoltaics and Renewable Energy Engineering, University of New South Wales

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: 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.

Date: 2017
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DOI: 10.1038/ncomms14120

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