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Phys Rev Lett. 2003 Jun 13;90(23):238305. Epub 2003 Jun 13.

Single-molecule photon counting statistics via generalized optical Bloch equations.

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  • 1Department of Chemistry and Biochemistry, University of California, Santa Barbara, CA 93106-9510, USA.


We derive the generating function for single molecule photon emission events within the context of the stochastically modulated optical Bloch equations. Statistical properties of single molecule photon counting experiments are deduced from a set of coupled differential equations only slightly more complicated than the Bloch equations themselves. This formulation allows for the study of photon bunching and antibunching within a single theoretical framework and provides a description of these behaviors that emphasizes the connection with single molecule experiments. Application is made to the spectroscopy of a chromophore coupled to a single two level system.

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