A single chromophore can only emit a maximum of one single photon per excitation cycle. This limitation results in a phenomenon commonly referred to as photon antibunching (pAB). When multiple chromophores contribute to the fluorescence measured, the degree of pAB has been used as a metric to "count" the number of chromophores.
View Article and Find Full Text PDFBy measuring the fluorescence photon statistics of single chains of a conjugated polymer, we determine the lifetime of the metastable dark state, the triplet exciton. The single molecule emits single photons one at a time, giving rise to photon antibunching. These photons appear bunched in time over longer time scales because of excursions to the triplet dark state.
View Article and Find Full Text PDFThe breaking of molecular symmetry through photoexcitation is a ubiquitous but rather elusive process, which, for example, controls the microscopic efficiency of light harvesting in molecular aggregates. A molecular excitation within a π-conjugated segment will self-localize due to strong coupling to molecular vibrations, locally changing bond alternation in a process which is fundamentally nondeterministic. Probing such symmetry breaking usually relies on polarization-resolved fluorescence, which is most powerful on the level of single molecules.
View Article and Find Full Text PDF