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Journal of Experimental and Theoretical Physics Letters

Photon distribution functions of the fluorescence photons from a single nanoparticle in various photon counting methods

Игорь Сергеевич Осадько

Published Aug 1, 2007• 11 citations
Publisher

Abstract

Simple expressions have been derived for three photon distribution functions w (T), w (T), and w (T) corresponding to three different methods for counting fluorescence photons from a single nanoparticle excited by continuous laser radiation. In contrast to the previously derived expressions represented in the form of N multiple integrals, the new expressions contain only single or double integrals of Poisson functions, which makes it possible to easily perform the numerical calculation of the photon distribution. The simplest photon counting method corresponds to the lengthiest function w (T); on the contrary, the simplest function w (T) corresponds to the most complex photon counting method. The functions w (T), w (T), and w (T) are noticeably different in short time intervals T; however, the distributions calculated using these functions are almost indistinguishable from each other in long T intervals. This circumstance makes it possible to use the simplest function w (T) to consider the photon statistics measured by the simplest method. This possibility is particularly important for investigating the fluorescence photon statistics, where the intensity fluctuates.

DOI
10.1134/s0021364007110057

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Simple expressions have been derived for three photon distribution functions w (T), w (T), and w (T) corresponding to three different methods for counting fluorescence photons from a single nanoparticle excited by continuous laser radiation. In contrast to the previously derived expressions represented in the form of N multiple integrals, the new expressions contain only single or double integrals of Poisson functions, which makes it possible to easily perform the numerical calculation of the photon distribution. The simplest photon counting method corresponds to the lengthiest function w (T); on the contrary, the simplest function w (T) corresponds to the most complex photon counting method. The functions w (T), w (T), and w (T) are noticeably different in short time intervals T; however, the distributions calculated using these functions are almost indistinguishable from each other in long T intervals. This circumstance makes it possible to use the simplest function w (T) to consider the photon statistics measured by the simplest method. This possibility is particularly important for investigating the fluorescence photon statistics, where the intensity fluctuates.
Distribution function w(N)(T) for photons created by three-level nanoparticle in time interval T under cw laser excitation is calculated for various methods of photon counting. It is found that each exponential process exp(-lambda(i)t) in quantum dynamics of three-level nanoparticle manifests itself via Poissonian function P(N)(lambda(i)t)=(lambda(i)t)(N) exp(-lambda(i)t)/N! in the photon distribution function w(N)(T). The distribution function w(N)(T) is expressed via two or three integrals of two or three Poissonian functions P(N)(lambda(i)t). The simple mathematical expression for w(N)(T) enables one to calculate photon distribution in blinking fluorescence with on and off intervals. A scaling between photon distribution function w(N)(T) and photoelectric pulse distribution function w(n)(T) is found. Comparison of the theoretical distribution w(n)(T) and the distribution measured in blinking fluorescence of single polymer molecule dPPV-PPyV and complex organic molecule 1,1(')-didodecyl-3,3,3('),3(')-tetramethylindocarbocyanine perchlorate (DiI) is carried out. The theoretical distributions are able to describe those found in an experiment.
Various methods of photon counting in single molecule blinking fluorescence are considered and photon distribution functions, , , and related to these methods are derived. It is shown that each exponential process exp(−λ j t) in quantum dynamics of a single molecule manifests itself in the mathematical expressions for the photon distribution function via Poissonian function PN (−λ j t) with the same rate constant. This relation enables one to avoid N-fold integration in the mathematical expressions for the functions, , , and derived in previous works. Numerical calculations of the functions , , and for blinking fluorescence are carried out. A relation between photon distribution and photo-electric pulse distribution is discussed. Thanks to relation found we can use photo-electric pulse distribution functions for studying photon distribution function and for studying quantum dynamics of single nanoparticle with blinking fluorescence.
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.
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.
We study the general properties of the photon statistics of fluorescence radiation, emitted by a two-level atom in a strong laser field and a perturber bath. We investigate the deviation of the factorial moments from a Poisson distribution, and we show that for long counting times the lowest-order correction can be expressed entirely by the quantity Q, which represents the deviation of the variance from the average. We introduce and evaluate the quantities gn(t), which serve as a measure for the deviation of the higher-order statistics from Poissonian statistics. Subsequently we obtain explicit expressions for the average waiting time for the appearance of the n th photon, after an arbitrary initialization of the counting process. It turns out that the average time delay is again determined by Q. Hence this parameter can be measured in a photon-counting experiment, which involves only the observation of a single photon, rather than an (in principle) infinite number of photons.