Effect of Thermal Fluctuations on the Radiative Rate in Core/Shell Quantum Dots.

The effect of lattice fluctuations and electronic excitations on the radiative rate is demonstrated in CdSe/CdS core/shell spherical quantum dots (QDs). Using a combination of time-resolved photoluminescence spectroscopy and atomistic simulations, we show that lattice fluctuations can change the radiative rate over the temperature range from 78 to 300 K. We posit that the presence of the core/shell interface plays a significant role in dictating this behavior. We show that the other major factor that underpins the change in radiative rate with temperature is the presence of higher energy states corresponding to electron excitation into the shell. These effects should be present in other core/shell samples and should also affect other excited state rates, such as the rate of Auger recombination or the rate of charge transfer.