Theory for Wavelength-Resolved Photon Emission Statistics in Single-Molecule Fluorescence Spectroscopy

Golan Bel and Frank L. H. Brown
Phys. Rev. Lett. 102, 018303 – Published 9 January 2009

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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  • Received 17 July 2008

DOI:https://doi.org/10.1103/PhysRevLett.102.018303

©2009 American Physical Society

Authors & Affiliations

Golan Bel* and Frank L. H. Brown

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

  • *Present address: Center for Nonlinear Studies, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.

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Vol. 102, Iss. 1 — 9 January 2009

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