Observation of Inverted Regime Electron Transfer in CdSe/ZnS QDs from pH-Sensitive Single-Particle and Ensemble Fluorescence Measurements

Abstract

In this report, we investigated the pH dependence of the photoluminescence of CdSe/ZnS quantum dots (QDs). We present experimental results and theoretical analysis of both the blinking behavior of single-QDs as well as the fluorescence intensity time trace from an ensemble of QDs in agarose gel fibers at different pH environments. Such a combined approach of confined QDs by single-particle and ensemble measurements has not been used previously. This study allows us to elucidate the electron transfer processes from the light state to the dark state. The observed increase in both the activation energy for the charge transfer and the free energy gap between the light and the dark states at an increased concentration of H(+) ions supported the Marcus inverted-regime, electron transfer.