Theory for Wavelength-Resolved Photon Emission Statistics in Single-Molecule Fluorescence Spectroscopy Academic Article uri icon

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.

publication date

  • January 9, 2009