Radiative and nonradiative recombination of photoexcited excitons in multi-shell-coated CdSe/CdS/ZnS quantum dots

Colloidal quantum dots (QDs) have been widely studied for nanophotonics and bioimaging applications for which the lifetime of their fluorescence is of critical importance. We report experimental and theoretical characterizations of dynamic optical properties of multi-shell-coated CdSe/CdS/ZnS QDs. Quantum-mechanical studies of fundamental optical excitations and Monte Carlo simulations of energy relaxation mechanisms indicate that the excitonic states are densely compacted in the QDs and are easily photoexcited by the laser pulse in the presence of nonradiative electron-phonon interactions. For spherical QDs, the decay time of spontaneous radiative emission of individual photoexcited excitonic states with zero angular momenta is found to be only tens of picoseconds. In our multi-shell QDs, high-energy excitonic states of nonzero angular momenta have to go through a number of nonradiative electron-phonon interaction steps in order to relax to zero-angular-momentum excitonic states for radiative emission, resulting in an effective fluorescence peak at about 2 ns in the photoncount-time relationship. This explains the measured long average fluorescence lifetime of 3.6 ns. Such a long lifetime facilitates the applications of colloidal QDs in areas such as QD-based solar cells, bioimaging and metamaterials. Copyright (c) EPLA, 2009