Mechanism of Single-Photon Upconversion Photoluminescence in All-Inorganic Perovskite Nanocrystals: The Role of Self-Trapped Excitons

Mechanism of Single-Photon Upconversion Photoluminescence in All-Inorganic Perovskite Nanocrystals: The Role of Self-Trapped Excitons

The efficient single-photon upconversion photoluminescence (UCPL) feature of lead halide perovskite semiconductors makes it promising for developing laser cooling devices. This is an attractive potential application, but the underlying physics still remains unclear so far. By using the all-inorganic...

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Veröffentlicht in:The journal of physical chemistry letters 2019-10, Vol.10 (20), p.5989-5996
Hauptverfasser: Ma, Xiaoman, Pan, Fang, Li, Haoqi, Shen, Peng, Ma, Chao, Zhang, Lei, Niu, Haibo, Zhu, Youzhang, Xu, Shijie, Ye, Honggang
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container_end_page 5996
container_issue 20
container_start_page 5989
container_title The journal of physical chemistry letters
container_volume 10
creator Ma, Xiaoman
Pan, Fang
Li, Haoqi
Shen, Peng
Ma, Chao
Zhang, Lei
Niu, Haibo
Zhu, Youzhang
Xu, Shijie
Ye, Honggang
description The efficient single-photon upconversion photoluminescence (UCPL) feature of lead halide perovskite semiconductors makes it promising for developing laser cooling devices. This is an attractive potential application, but the underlying physics still remains unclear so far. By using the all-inorganic CsPbX3 (X = Br, I) nanocrystal samples, this phenomenon was investigated by photoluminescence (PL) and time-resolved PL under different temperatures and various excitation conditions. A broad emission band located at the low-energy side of the free exciton (FE) peak was detected and deduced to be from the self-trapped exciton (STE). The lifetime of STE emission was found to be 171 ns at 10 K, much longer than that of FE. The UCPL phenomenon was then attributed to thermal activation of transformation from STEs to FEs, and the energy barrier was derived to be 103.7 meV for CsPbBr3 and 45.2 meV for CsPb­(Br/I)3, respectively. The transformation also can be seen from the fluorescence decay processes.
doi_str_mv 10.1021/acs.jpclett.9b02289
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title Mechanism of Single-Photon Upconversion Photoluminescence in All-Inorganic Perovskite Nanocrystals: The Role of Self-Trapped Excitons
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