Unraveling the exciton quenching mechanism of quantum dots on antimony-doped SnO_2 films by transient absorption and single dot fluorescence spectroscopy

摘要

Integrating quantum dots (QDs) into modern optoelectronic devices requires an understanding of how a transparent conducting substrate affects the properties of QDs, especially their excited-state dynamics. Here, the exciton quenching dynamics of core/multishell (CdSe/CdS_(3ML)ZnCdS _(2ML)ZnS_(2ML)) quantum dots deposited on glass, tin oxide (SnO_2), and antimony (Sb)-doped tin oxide (ATO) films are studied by transient absorption and single QD fluorescence spectroscopic methods. By comparing ensemble-averaged fluorescence decay and transient absorption kinetics, we show that, for QDs on SnO_2, the exciton is quenched by electron transfer from the QD to SnO2. At the QD-ATO interface, much faster exciton quenching rates are observed and attributed to fast Auger recombination in charged QDs formed by Fermi level equilibration between the QD and n-doped ATO. Single QDs on SnO_2 and ATO show similar blinking dynamics with correlated fluctuations of emission intensities and lifetimes. Compared to QDs on SnO2, QDs on ATO films show larger variation of average exciton quenching rates, which is attributed to a broad distribution of the number of charges and nature of charging sites on the QD surface.