Revealing single emitter spectral dynamics from intensity correlations in an ensemble fluorescence spectrum

We show that the single emitter linewidth underlying a broadened ensemble emission spectrum can be extracted from correlations among the stochastic intensity fluctuations in the ensemble spectrum. Spectral correlations can be observed at high temporal and spectral resolutions with a cross-correlated pair of avalanche photodiodes placed at the outputs of a scanning Michelson interferometer. As illustrated with simulations in conjunction with Fluorescence Correlation Spectroscopy, our approach overcomes ensemble and temporal inhomogeneous broadening to provide single emitter linewidths, even for emitters under weak, continuous, broadband excitation. (C) 2009 Optical Society of America