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By performing spectroscopic single-particle measurements at cryogenictemperatures over the course of hours we study %By performing spectroscopiclongtime single-particle measurements at cryogenic temperatures we study boththe spectral diffusion as well as the diffusion of the decay rates of thefluorescence emission of core/shell CdSe/CdS dot/rod nanoparticles. A specialanalysis of the measurements allow for a correlation of data for single neutralexcitons only, undisturbed by the possible emission of other excitoniccomplexes. We find a nearly linear dependency of the fluorescence decay rate onthe emission energy. The experimental data is compared to self-consistent modelcalculations within the effective-mass approximation, in which migrating pointcharges set onto the surface of the nanoparticles have been assumed to causethe temporal changes of optical properties. These calculations reveal a nearlylinear relationship between the squared electron-hole wave function overlap,which is linked to the experimentally determined fluorescence rate, and theexciton emission energy. Within our model single migrating surface charges arenot sufficient to fully explain the measured rather broad ranges of emissionrates and energies, while two -- and in particular negative -- surface chargesclose to the core of the DR induce large enough shifts. Importantly, for ournanoparticle system, the surface charges more strongly affect the hole wavefunction than the electron wave function and both wave functions are stilllocalized within the dot-like core of the nanoparticle, showing that the type-Icharacter of the band alignment between core and shell is preserved.

Surface Charges on CdSe-Dot/CdS-Rod Nanocrystals: Measuring and Modeling the Diffusion of Exciton-Fluorescence Rates and Energies