Abstract
By severely reducing the number of solute molecules in the illuminated sample, the optical resonances of individual molecules can be resolved in a fluorescence excitation spectrum. Single molecule lines can be studied as a function of time and temperature: sudden jumps of their resonance frequencies are due to spectral diffusion processes. The signal from a single molecule displays specific correlations which makes time-resolved studies possible. Here, emphasis is put on photon-bunching arising from intersystem crossing (ISC). ISC rates are deduced from the observed decay rates of the correlation and are found to differ from molecule to molecule. A single molecule is a truly local probe of its environment by means of which fundamental studies of the matrix dynamics as well as nanophysics experiments may be undertaken.
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