Citation: Rongliang Deng, Yihang Chen, Xiaotong Fan, Guolong Chen, Shuli Wang, Changzhi Yu, Xiao Yang, Tingzhu Wu, Zhong Chen, Yue Lin. Break of thermal equilibrium between optical and acoustic phonon branches of CsPbI₃ under continuous-wave light excitation and cryogenic temperature[J]. Chinese Chemical Letters, ;2024, 35(7): 109346. doi: 10.1016/j.cclet.2023.109346 shu

Break of thermal equilibrium between optical and acoustic phonon branches of CsPbI₃ under continuous-wave light excitation and cryogenic temperature

Rongliang Deng ^{a, 1} ,
Yihang Chen ^{a, 1} ,
Xiaotong Fan ^a ,
Guolong Chen ^a ,
Shuli Wang ^a ,
Changzhi Yu ^a ,
Xiao Yang ^{a, c} ,
Tingzhu Wu ^{a, b} ,
Zhong Chen ^{a, b} ,
Yue Lin ^{a, b, *,}

a.
Department of Electronic Science, Fujian Engineering Research Center for Solid-State Lighting, Xiamen University, Xiamen 361005, China
b.
Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361102, China
c.
Institute of Electromagnetics and Acoustics, School of Electronic Science and Engineering, Xiamen University, Xiamen 361005, China

yue.lin@xmu.edu.cn

Received Date: 10 October 2023
Revised Date: 13 November 2023
Accepted Date: 27 November 2023
Available Online: 7 December 2023

Figures(3)

The kinetic of low-temperature carrier and lattice of lead-halide perovskite is yet to be fully understood. In this work, we investigate the steady-state photoluminescences (PLs) of CsPbI₃ at the environmental temperature (T_e) ranging from 20 K to 300 K, and observed anomalous behaviors at cryogenic temperatures: The carrier temperature (T_c) of pure CsPbI₃ exhibits a negative correlation with T_e, accompanied by an expansion in Urbach tails of absorption spectra (Abs.) and excessive red-shifts at peak energy of PLs. These phenomena are also observed in those samples containing a certain amount of Cs₄PbI₆, but to a lesser extent and occurs at lower temperatures. It is attributed to the intensified hot phonon bottleneck effect (HPB) in CsPbI₃ at cryogenic T_e, which hinders the energy transfer from hot carriers, via longitudinal optics (LO) phonons to longitudinal acoustic (LA) phonons, to the ambient. For samples under continuous-wave laser excitation, in specific, the barrier induced by the enhanced HPB at low T_e prevents the effective thermalization among carriers, LO and LA phonons, which, therefore, form thermally isolated ensembles with different temperatures. At cryogenic T_e range, the elevated temperatures of carrier and LO phonon expand the high-energy side of PLs and the low-energy tail of Abs., respectively. For those samples in which the CsPbI₃ is mixed with Cs₄PbI₆, the interfacial LO-LO interaction across them provides a bypass for heat dissipation, mitigating the heat accumulation in LO-phonons of CsPbI₃. The results suggest that a strong HPB effect may break the thermal equilibrium among different branches of phonons in the lattice under certain extreme conditions.
- CsPbI₃,
- Cs₄PbI₆,
- Low-temperature carrier,
- Lattice kinetic,
- Hot phonon bottleneck effect,
- Interfacial LO-LO interaction
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Break of thermal equilibrium between optical and acoustic phonon branches of CsPbI3 under continuous-wave light excitation and cryogenic temperature

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通讯作者: 陈斌, bchen63@163.com

Break of thermal equilibrium between optical and acoustic phonon branches of CsPbI₃ under continuous-wave light excitation and cryogenic temperature