Photonic mode density effects on single-molecule fluorescence blinking

Abstract

We investigated the influence of the photonic mode density (PMD) on the triplet dynamics of individual chromophores on a dielectric interface by comparing their response in the presence and absence of a nearby gold film. Lifetimes of the excited singlet state were evaluated in order to measure directly the PMD at the molecule's position. Triplet state lifetimes were simultaneously determined by statistical analysis of the detection time of the fluorescence photons. The observed singlet decay rates are in agreement with the predicted PMD for molecules with different orientations. The triplet decay rate varies in a fashion correlated to the singlet decay rate. These results show that PMD engineering can lead to an important suppression of the fluorescence blinking, introducing a novel physical mechanism to enhance fluorescence intensity in PMD-enhancing systems such as plasmonic devices.