Theory for wavelength-resolved photon emission statistics in single-molecule fluorescence spectroscopy.
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.
Bel
Golan
G
Department of Chemistry and Biochemistry and Department of Physics, University of California, Santa Barbara, California 93106, USA.
Brown
Frank L H
FL