Issue 17, 2022

Hot carrier relaxation in CsPbBr3 nanocrystals: electron–hole asymmetry and shape effects

Abstract

Optimization of the optoelectronic performance of lead halide perovskite (LHP) nanocrystals calls for understanding and manipulation of their hot carrier relaxation processes. In this work, the hot carrier relaxation in a nanocube (NC) and a nanoplate (NPL) of CsPbBr3 is studied using non-adiabatic molecular dynamics based on first-principles calculations. Strong electron–hole asymmetry in the relaxation processes is observed. Regardless of the nanocrystal shape, the hot hole cooling rate is much faster than that of hot electrons. Moreover, while the hot-hole relaxation is insensitive to the excitation energy, faster relaxation of hot electrons is observed with a lower excitation energy. The origin of the asymmetry is associated with the orbital characters and density of states at the band edges. The hot-hole relaxation is strongly affected by the shape of the nanocrystal. It is faster in the NPL than in the NC. This is attributed to the larger atomic displacements in the NPL due to its higher surface/volume ratio. These results provide theoretical insights for fundamental understanding of excited-state dynamics in LHPs and may help the development of hot-carrier optoelectronic devices.

Graphical abstract: Hot carrier relaxation in CsPbBr3 nanocrystals: electron–hole asymmetry and shape effects

Article information

Article type
Paper
Submitted
08 fev 2022
Accepted
31 mar 2022
First published
31 mar 2022

Phys. Chem. Chem. Phys., 2022,24, 9891-9896

Hot carrier relaxation in CsPbBr3 nanocrystals: electron–hole asymmetry and shape effects

Q. Gao and J. Kang, Phys. Chem. Chem. Phys., 2022, 24, 9891 DOI: 10.1039/D2CP00634K

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