Ultrafast Spectral Dynamics of CsPb(Br_xCl_1–x)₃ Mixed-Halide Nanocrystals

Abstract

In this study we investigated the spectral dynamics of cesium lead mixed-halide, CsPb(Br_<em>x</em>Cl_{1–<em>x</em>})₃ perovskite nanocrystals probed with complementary spectral techniques: time-resolved photoluminescence and transient absorption spectroscopy. Mixed-halide perovskite nanocrystals were synthesized via a hot-injection method followed by anion exchange reactions. Our results show that increased Cl content in perovskite nanocrystals (a) diminished the photoluminescence quantum yield and gave rise to rapid radiative recombination of carriers; (b) resulted in rapid thermalization of hot carriers and low carrier temperatures, which suggests weaker hot-phonon bottleneck and Burstein–Moss effects; (c) decreased the bandgap renormalization energy, which suggests high exciton binding energy and poor charge extraction in Cl substituted perovskite nanocrystals; and (d) increased the number of carriers undergoing Auger losses, where Auger processes dominate over trap-assisted recombination. Furthermore, these findings provide a generalized framework to guide researchers as to when mixed-halide perovskite nanocrystals would be useful for optoelectronic technologies and when they would be detrimental to device performance.