Temperature and Size Dependence of the Optical Properties of Tetrapod-Shaped Colloidal Nanocrystals Exhibiting Type-II Transitions

We have investigated the optical properties of colloidal seed-grown CdSe (seed)/CdTe (arms) nanotetrapods both experimentally and computationally. The tetrapods exhibit a type-II transition arising from electrons localized in the CdSe seed region and holes delocalized in the CdTe arms, along with a residual type-I recombination in long-arm tetrapods. Experiments and theory helped to identify the origin of both types of transitions and their size dependence. In particular, timeresolved experiments performed at 10 K evidenced a sizedependent, long living type-II radiative emission arising from the peculiar electron-hole wave function localization. Temperature- dependent photoluminescence (PL) studies indicate that, at high temperature (>150 K), the main process limiting the PL quantum efficiency of the type-I PL is thermal escape of the charge carriers through efficient exciton-optical phonon coupling. The type-II PL instead is limited both by thermal escape and by the promotion of electrons from the conduction band of the seed region to that of the arms, occurring at T > 200 K.