Size-dependent oscillator strength and quantum efficiency of CdSe quantum dots controlled via the local density of states

We study experimentally time-resolved emission of colloidal CdSe quantum dots in an environment with a controlled local density of states (LDOS). The decay rate is measured versus frequency and as a function of distance to a mirror. We observe a linear relation between the decay rate and the LDOS, allowing us to determine the size-dependent quantum efficiency and oscillator strength. We find that the quantum efficiency decreases with increasing emission energy mostly due to an increase in nonradiative decay. We manage to obtain the oscillator strength of the important class of CdSe quantum dots. The oscillator strength varies weakly with frequency in agreement with behavior of quantum dots in the strong confinement limit. Surprisingly, previously calculated tight-binding results differ by a factor of 5 with the measured absolute values. Results from pseudopotential calculations agree well with the measured radiative rates. Our results are relevant for applications of CdSe quantum dots in spontaneous emission control and cavity quantum electrodynamics.

• View at Publisher