Exciton Dynamics in Colloidal CdS Quantum Dots with Intense and Stokes Shifted Photoluminescence in a Single Decay Channel.

Abstract

CdS quantum dots (QDs), synthesized by a sol-gel method, exhibit significantly Stokes shifted bright photoluminescence (PL), predominantly from the trap states. Surprisingly, the PL decay at the emission maximum is single-exponential. This is an unusual observation for as-prepared QDs and indicates a narrow distribution in the nature of trap states. A closer look reveals an additional fast component for the decays at shorter emission wavelengths, presumably due to the band edge emission, which remains elusive in the steady-state spectra. Indeed, a significantly narrower and blue-shifted emission band is observed in the decay-associated spectra. The contribution of this component to the steady-state PL intensity is shown to be overwhelmed by that of the significantly stronger trap emission. Exciton dynamics in the quantum dots is elucidated using transient absorption spectra, in which the stimulated emission is observed even at low pump power.