Magnetic-field-dependent spin decoherence and dephasing in room-temperature CdSe nanocrystal quantum dots

We perform and analyze a series of time-resolved Faraday rotation measurements of coherent spin dynamics in a room-temperature ensemble of CdSe nanocrystal quantum dots (NCQDs) to study the decoherence and dephasing mechanisms that limit the transverse spin lifetime. Coherent spin lifetimes on the order of nanoseconds have been previously observed in CdSe NCQDs, but the presence of multiple components with distinct dynamics and strong inhomogeneous dephasing have made it difficult to study the relevant spin decay mechanisms quantitatively. Here, we obtain reliable fitting results by ensuring that cross-correlations between model parameters are minimized for the parameters of interest. Furthermore, we characterize the morphological inhomogeneity of the NCQD ensemble using transmission electron microscopy to constrain the model parameters that specify inhomogeneous dephasing. We find that g-factor inhomogeneity-induced dephasing (gID) is not sufficient to explain the magnetic-field-dependent decay of the spin signal. We propose an additional decoherence mechanism arising from rapid transitions between the fine structure states of the exciton referred to as fine-structure decoherence (FSD). By including both gID and FSD in the model, excellent fits are obtained to the data, including a prominent short-time-scale feature, which has typically been excluded from the fits in previous work.