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arXiv:quant-ph/0312084 · New Journal of Physics

Photon statistics characterization of a single-photon source

Romain Alléaume, François Treussart, Jean-Michel Courty, Jean-François Roch

Published Jul 30, 2004• 60 citations
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Abstract

In a recent experiment, we reported the time-domain intensity noise measurement of a single-photon source relying on single-molecule fluorescence control. In this paper, we present data processing starting from photocount timestamps. The theoretical analytical expression of the time-dependent Mandel parameter Q ( T ) of an intermittent single-photon source is derived from ON↔OFF dynamics. Finally, source intensity noise analysis, using the Mandel parameter, is quantitatively compared with the usual approach relying on the time autocorrelation function, both methods yielding the same molecular dynamical parameters.

DOI
10.1088/1367-2630/6/1/085

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In a recent experiment, we reported the time-domain intensity noise measurement of a single-photon source relying on single-molecule fluorescence control. In this paper, we present data processing starting from photocount timestamps. The theoretical analytical expression of the time-dependent Mandel parameter Q ( T ) of an intermittent single-photon source is derived from ON↔OFF dynamics. Finally, source intensity noise analysis, using the Mandel parameter, is quantitatively compared with the usual approach relying on the time autocorrelation function, both methods yielding the same molecular dynamical parameters.
We studied intensity fluctuations of a single photon source relying on the pulsed excitation of the fluorescence of a single molecule at room temperature. We directly measured the Mandel parameter Q(T) over 4 orders of magnitude of observation time scale T by recording every photocount. On time scale of a few excitation periods, sub-Poissonian statistics is clearly observed and the probablility of two-photons events is 10 times smaller than Poissonian pulses. On longer times, blinking in the fluorescence, due to the molecular triplet state, produces an excess of noise.
The lack of reliable quantitative methods in fluorescence microscopy prevents the detailed investigation of basic molecular processes. Single-molecule fluorescence spectroscopy offers several techniques to determine the stoichiometry of fluorescent probes. Among them, an approach using the single-photon emission of an individual quantum system, also known as photon antibunching, yields access to both the emitter number and their molecular brightness. Previous work demonstrated the feasibility of the method to estimate up to five dyes without further physical characterization. In this work, I investigated and improved the reliability and robustness of this method. I developed different fluorescent probes with a defined label stoichiometry to explore the performance of our approach \nin experiments. I could demonstrate, in combination with simulations, that it can provide reliable estimates of up to 18 fluorescent emitters at a time resolution of approximately 200 ms. Furthermore, I inspected the dependency of the estimation bias and precision on the laser intensity, the analysis time and the number of expected molecules in detail. My results designate the scope for future stoichiometry determinations. In initial experiments, I analyzed the labeling distributions of different fluorescent probes. In addition, I could combine our counting approach with super-resolution STED-microscopy and identify critical parameters for possible applications
We theoretically study the photon counting statistics characterizations of the real single molecular photon source with a Poisson statistics background and that of an ideal double molecular system based on the standard HBT detection. Mandel parameter Q of each source with the same mean photons n—was analyzed. We have obtained an efficient method to identify single molecule by the two-photon statistics probability P(2), which shows the relation P(2)2. Additionally, we studied the effect of single-to-background ratio of the single molecular photon source on the criterion.
We studied the photon statistics of the driven single molecule under intersystem crossing process which caused the fluorescence blinking via generating function approach.We give an analytical expression of the average emission photons N and the Mandel's Q parameter in long time limit.The results demonstrate that the Mandel's Q parameter has the same behavior as the average emission photons N with respect to the evolution time,both of them linearly increasing with the evolution time increase,when the intersystem crossing process occurred in the single molecule.
We theoretically derive exact expressions for Mandel's Q parameter of the triggered single molecular source, which is inferred from the probabilities P RS ( n ) using the record of each photon detection event based on Hanbury Brown and Twiss detection. The real triggered source is recognized as an ideal single photon source with a Poissonian statistics background. How to decrease the background and to increase the efficiency are discussed. It is established that the sub-Poissonian statistics formation can be determined by comparing the measured Q RS of the real single triggered molecular with Q C of the Poissonian source containing the same mean photons. By this method, we also give an efficient way to measure signal-to-background ratios of triggered single photons.
We theoretically derive exact expressions for Mandel's Q parameter of the triggered single molecular source, which is inferred from the probabilities PRs (n) using the recorded of each photon detection event based on Hanbury Brown and Twiss detection. The real triggered source is recognized as an ideal single photon source with a Poissonian statistics background. How to decease the background and to increase the efficiency are discussed. It is established that the sub-Poissonian statistics formation can be determined by comparing the measured QRs of the real single triggered molecular with Qc of the Poissonian source containing the same mean photons. By this method, we also give an efficient way to measure signal-to-background ratios of triggered single photons.