Biexciton Dynamics in Single Colloidal CdSe Quantum Dots

The investigation of biexciton dynamics in single colloidal quantum dots (QDs) is critical to biexciton-based applications. Generally, a biexciton exhibits an extremely low photoluminescence (PL) quantum yield as well as very fast PL decay due to strong nonradiative Auger recombination, making it difficult to investigate the biexciton dynamics. Here, we develop a quantitative method based on intensity- and time-resolved photon statistics to investigate the biexciton dynamics in single colloidal QDs. This robust method can be used under high-excitation conditions to determine the absolute radiative and Auger recombination rates of both neutral and charged biexciton states in a single QD level, and the corresponding ratios between the two states agree with the theoretical predictions of the asymmetric band structures of CdSe-based QDs. Furthermore, the surface traps are found to provide additional nonradiative recombination pathways for the biexcitons, and their contributions are quantified by the method.