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Journal of Experimental and Theoretical Physics

Sub-poissonian statistics of fluorescence from a single atom driven by a continuous wave laser field

Игорь Сергеевич Осадько

Published Jul 1, 2005• 14 citations
Publisher

Abstract

Statistics of fluorescence photons emitted by a single two-level atom interacting with a continuous wave laser field are analyzed. The photon-counting distribution is calculated for the so-called intermediate fluorescence photons, i.e., those counted during the time interval between instants at which photons are emitted. The result is a sub-Poissonian (narrower than Poisson) distribution, which agrees with experimental observations. This intermediate-photon distribution is used to calculate the average number of fluorescence photons, the second factorial moment of the photon-counting distribution, and Mandel’s Q parameter commonly used to evaluate the deviation of photon statistics from the Poisson distribution. The theoretical expressions obtained for moments of the intermediate-photon distribution are different from well-known Mandel’s formulas.

DOI
10.1134/1.2010662

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Statistics of fluorescence photons emitted by a single two-level atom interacting with a continuous wave laser field are analyzed. The photon-counting distribution is calculated for the so-called intermediate fluorescence photons, i.e., those counted during the time interval between instants at which photons are emitted. The result is a sub-Poissonian (narrower than Poisson) distribution, which agrees with experimental observations. This intermediate-photon distribution is used to calculate the average number of fluorescence photons, the second factorial moment of the photon-counting distribution, and Mandel’s Q parameter commonly used to evaluate the deviation of photon statistics from the Poisson distribution. The theoretical expressions obtained for moments of the intermediate-photon distribution are different from well-known Mandel’s formulas.
An analysis of intermittent fluorescence is presented for a single molecule driven by a continuous-wave laser field. The interruptions of fluorescence are caused by transition of the molecule to a triplet state. A method previously developed to calculate photon distribution for continuous-wave fluorescence is applied to analyze photon statistics of fluorescence blinking. The probability w N (T) of counting N photons over a time interval T is derived for intermittent fluorescence. The photons counted over relatively short intervals are found to have a sub-Poissonian (narrower than Poisson) distribution. The photon distribution over intervals longer than the mean off time has a complicated form with two maxima; i.e., a super-Poissonian (wider than Poisson) distribution is obtained.
The method previously used by the author for the measurement and calculation of the distribution function w N(T)of fluorescence photons from a single two-level atom that is continuously excited by laser light and has a unity fluorescence quantum yield is generalized to the case of a single molecule whose fluorescence quantum yield is smaller than unity and to the case of a three-level molecule whose fluorescence is blinking. The functions w N(T) calculated for these two cases demonstrate a sub-Poissonian distribution of fluorescence photons.
Abstract Measurement of photon statistics is an important tool for the verification of quantum properties of light. Due to the various imperfections of real single photon detectors, the observed statistics of photon counts deviates from the underlying statistics of photons. Here we analyze statistical properties of coherent states, and investigate a connection between Poissonian distribution of photons and sub-Poissonian distribution of photon counts due to the detector dead-time corrections. We derive a functional dependence between the mean number of photons and the mean number of photon counts, as well as connection between higher-order statistical moments, for the pulsed or continuous wave coherent light sources, and confirm the results by numerical simulations.
We investigate the distribution of the number of photons emitted by a single molecule undergoing a spectral diffusion process and interacting with a continuous wave laser field. The spectral diffusion is modeled based on a stochastic approach, in the spirit of the Anderson-Kubo line shape theory. Using a generating function formalism we solve the generalized optical Bloch equations and obtain an exact analytical formula for the line shape and Mandel's Q parameter. The line shape exhibits well-known behaviors, including motional narrowing when the stochastic modulation is fast and power broadening. The Mandel parameter, describing the line shape fluctuations, exhibits a transition from a quantum sub-Poissonian behavior in the fast modulation limit to a classical super-Poissonian behavior found in the slow modulation limit. Our result is applicable for weak and strong laser fields, namely, for arbitrary Rabi frequency. We show how to choose the Rabi frequency in such a way so that the quantum sub-Poissonian nature of the emission process becomes strongest. A lower bound on Q is found and simple limiting behaviors are investigated. A nontrivial behavior is obtained in the intermediate modulation limit, when the time scales for spectral diffusion and the lifetime of the excited state become similar. A comparison is made between our results and previous ones derived, based on the semiclassical generalized Wiener-Khintchine formula.