Multiexciton dynamics in CsPbBr3 nanocrystals: the dependence on pump fluence and temperature

Abstract

Multiexcitons generation is a process of generating electron–hole pairs in nanostructured semiconductors by absorbing a single high-energy photon. The multiexciton process is essential for the performance of optoelectronic devices based on perovskite nanomaterials. In this paper, ultrafast time-resolved transient absorption spectroscopy is used to study the ultrafast dynamics of CsPbBr3 nanocrystals. It is found that the multiexcitons Auger recombination lifetime increases with the decrease of pump fluence, while it is on the contrary for the hot carrier cooling time. The increase in the number of photons absorbed by each nanocrystal under high pump fluence slows down the relaxation of hot carriers to the band edge. The hot carrier cooling lifetime increases from 0.25 to 0.85 ps when the pump fluence increases from 6 to 127 μJ cm−2. Temperature-dependent transient absorption spectroscopy exhibits that the relaxation process of hot carriers slows down sharply when the lattice temperature decreases from 280 to 80 K. Moreover, the exciton binding energy 46 meV of CsPbBr3 nanocrystals is obtained by temperature-dependent steady-state photoluminescence spectroscopy. These findings provide insights for applications such as solar cells and light-emitting devices based on CsPbBr3 nanocrystals.