Photon antibunching in a cluster of giant CdSe/CdS nanocrystals

When closely packed into a high-density film, semiconductor nanocrystals (NCs) can interact with each other to yield collective optical behaviours, which are normally difficult to characterize due to the ensemble average effect. Here we synthesized semiconductor NC clusters and performed single-particle spectroscopic measurements to probe the electronic couplings of several giant CdSe/CdS NCs contained in one cluster with nanometer-scale separations. Such a single cluster exhibits multiple emission peaks at the cryogenic temperature with nearly identical photoluminescence decay dynamics, suggesting that the Förster-type energy transfer does not occur among the composing NCs. Surprisingly, strong photon antibunching is still observed from a single cluster, which can be attributed to the Auger annihilation of photo-excited excitons from different NCs. The isolation of several nearby NCs interacting with the above novel mechanism has marked a solid progress towards a full understanding and an efficient control of the operation parameters in NC-based optoelectronic devices.