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Title: Theory of single molecule emission spectroscopy

A general theory and calculation framework for the prediction of frequency-resolved single molecule photon counting statistics is presented. Expressions for the generating function of photon counts are derived, both for the case of naive “detection” based solely on photon emission from the molecule and also for experimentally realizable detection of emitted photons, and are used to explicitly calculate low-order photon-counting moments. The two cases of naive detection versus physical detection are compared to one another and it is demonstrated that the physical detection scheme resolves certain inconsistencies predicted via the naive detection approach. Applications to two different models for molecular dynamics are considered: a simple two-level system and a two-level absorber subject to spectral diffusion.
Authors:
 [1] ;  [2] ;  [2] ;  [3]
  1. Department of Solar Energy and Environmental Physics, Jacob Blaustein Institutes for Desert Research, Ben-Gurion University of the Negev, Sede Boqer Campus 84990 (Israel)
  2. (United States)
  3. Department of Chemistry and Biochemistry and Department of Physics, University of California, Santa Barbara, California 93106 (United States)
Publication Date:
OSTI Identifier:
22415733
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 17; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COMPARATIVE EVALUATIONS; DETECTION; DIFFUSION; EMISSION SPECTROSCOPY; MOLECULAR DYNAMICS METHOD; MOLECULES; PHOTON EMISSION; PHOTONS