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Phys Rev Lett. 2009 Jan 9;102(1):018303. Epub 2009 Jan 9.

Theory for wavelength-resolved photon emission statistics in single-molecule fluorescence spectroscopy.

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1
Department of Chemistry and Biochemistry and Department of Physics, University of California, Santa Barbara, California 93106, USA.

Abstract

We derive the moment generating function for photon emissions from a single molecule driven by laser excitation. The frequencies of the fluoresced photons are explicitly considered. Calculations are performed for the case of a two-level dye molecule, showing that measured photon statistics will display a strong and nonintuitive dependence on detector bandwidth. Moreover, it is demonstrated that the antibunching phenomenon, associated with negative values of Mandel's Q parameter, results from correlations between photons with well separated frequencies.

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