Charge hopping revealed by jitter correlations in the photoluminescence spectra of single CdSe nanocrystals

Spectral fluctuations observed in single CdSe/ZnS nanocrystals at 5 K are found to be entirely the result of discrete charge hops in the local environment of the nanocrystal, which occur at a rate comparable to the acquisition time of a single spectrum. We show that intervals between discrete spectral hops introduce a correlation between the successive measurements of the emission wavelength of single CdSe nanocrystals. This correlation can be recovered even in the presence of noise, but is shown to be sensitive to the experimental acquisition time, in good agreement with theory. However, we only find correlations for the smaller of the two nanocrystal sizes studied and discuss this in terms of size-dependent time scales correlated with the amount of excess energy dissipated in the nanocrystal due to hot-carrier relaxation.