Trion-Facilitated Dexter-Type Energy Transfer in a Cluster of Single Perovskite CsPbBr₃ Nanocrystals

Semiconductor colloidal nanocrystals (NCs) can interact with each other to profoundly influence the charge transfer, transport and extraction processes after they have been assembled into a high-density film for optoelectronic device applications. These interactions normally occur among several nearby single colloidal NCs, which should be effectively separated from their surroundings to remove the ensemble average effect for fine optical characterizations. By means of atomic force microscopy (AFM) nanoxerography, here we prepare individual clusters of perovskite CsPbBr₃ NCs and perform single-particle measurements on their optical properties at the cryogenic temperature. While discrete photoluminescence bands can be resolved from the several single CsPbBr₃ NCs that are contained within an individual cluster, the shorter- and longer-wavelength bands are dramatically different in that their intensities show sub- and superlinear dependences on the laser excitation powers, respectively. This can be explained by the generation of charged excitons (trions) at high laser excitation powers, and their subsequent Dexter-type energy transfer from smaller- to larger-sized CsPbBr₃ NCs. Our findings not only suggest that these individual clusters prepared by AFM nanoxerography can serve as a potent platform to explore few-NC interactions but they also reveal the long-neglected role played by trions in channeling photo-excited energies among neighboring NCs. (paper)