Composition‐Dependent Hot Carrier Relaxation Dynamics in Cesium Lead Halide (CsPbX₃, X=Br and I) Perovskite Nanocrystals

Abstract

Cesium-based perovskite nanocrystals (NCs) have outstanding photophysical properties improving the performances of lighting devices. Fundamental studies on excitonic properties and hot-carrier dynamics in perovskite NCs further suggest that these materials show higher efficiencies compared to the bulk form of perovskites. However, the relaxation rates and pathways of hot-carriers are still being elucidated. By using ultrafast transient spectroscopy and calculating electronic band structures, we investigated the dependence of halide in Cs-based perovskite (CsPbX₃ with X=Br, I, or their mixtures) NCs on the hot-carrier relaxation processes. All samples exhibit ultrafast (<0.6 ps) hot-carrier relaxation dynamics with following order: CsPbBr₃ (310 fs)>CsPbBr_1.5 I_1.5 (380 fs)>CsPbI₃ NC (580 fs). These result accounts for a reduced light emission efficiency of CsPbI₃ NC compared to CsPbBr₃ NC.