Reduction of Optical Gain Threshold in CsPbI₃ Nanocrystals Achieved by Generation of Asymmetric Hot-Biexcitons

Lead halide perovskite nanocrystals (NCs) are a class of promising light-emitting materials and have been considered as gain media in lasers. Strong exciton-exciton interactions in NCs cause an energy shift of the lowest optical transition and affect the optical gain threshold. Here, we clarify the dynamics of exciton-exciton interactions in highly photoexcited CsPbI₃ NCs by double-pump transient absorption spectroscopy. This method provides control over the population of each excited state by varying the time interval between the two pump pulses. We find that the band-edge energy shift induced by the formation of asymmetric hot-biexcitons (comprising one ground-state exciton and one hot exciton) is smaller than that induced by hot excitons and hot biexcitons in the ensemble. We demonstrate that the generation of asymmetric hot-biexcitons reduces the optical gain threshold in the CsPbI₃ NC ensemble.