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Physical Review Letters

Nonclassical Photon Statistics in Single-Molecule Fluorescence at Room Temperature

L. Fleury, Jean‐Manuel Segura, G. Zumofen, Bert Hecht, Urs P. Wild

Published Feb 7, 2000• 254 citations
Publisher

Abstract

The fluorescence of single terrylene molecules in a crystalline host is investigated at room temperature by scanning confocal optical microscopy. Photon arrival times are analyzed in terms of interphoton time distributions, second order correlation functions, and the variance of the photon number probability distribution. Antibunching at short times and bunching behavior for longer times is observed, associated with sub- and super-Poissonian statistics, respectively. A rate-equation analysis of the molecular level populations indicates an accelerated reverse intersystem crossing.

DOI
10.1103/physrevlett.84.1148

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The fluorescence of single terrylene molecules in a crystalline host is investigated at room temperature by scanning confocal optical microscopy. Photon arrival times are analyzed in terms of interphoton time distributions, second order correlation functions, and the variance of the photon number probability distribution. Antibunching at short times and bunching behavior for longer times is observed, associated with sub- and super-Poissonian statistics, respectively. A rate-equation analysis of the molecular level populations indicates an accelerated reverse intersystem crossing.
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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.
Fluorescence photons emitted by a single molecule trapped in a solid at low temperature are correlated in time. A simple theory of the correlation pattern is presented, including in the same formalism photon antibunching from coherent Rabi oscillations and photon bunching due to incoherent quantum transitions between electronic levels. The correlation method is applied to single pentacene molecules in a para-terphenyl crystal. A clear photon bunching allows us to determine the ISC rates for each molecule. We attribute the scatter of our results for the transition rate between excited singlet and triplet states, and the difference with the average value taken from the literature, to molecular distortions induced by crystal defects in our small sample. We conclude that the correlation method associated to single molecule spectroscopy has a great potential to study dynamical processes on intermediate time scales in condensed matter.
Photon emission from a single molecule at room temperature exhibits nonclassical features. Continuous wave fluorescence excitation provides antibunching in the emitted photons sequence as a signature of the property to only emit one photon at a time. A short pulsed excitation can then produce single photons on demand, with an overall quantum efficiency up to 4.5% in our experimental setup. Direct measurement of the Mandel parameter Q ( T ) for an observation period of duration T follows a subpoissonian statistics on short time scale and superpoissonian statistics on longer time scale. The latter is attributed to blinking in the fluorescence due to the occurence of a metastable molecular triplet state.
The fluorescence of single colloidal CdSe quantum dots is investigated at room temperature by means of the autocorrelation function over a time scale of almost 12 orders of magnitude. At short time, the autocorrelation function shows a complete antibunching indicating single photon emission and atomic-like behavior. On longer time scales (up to tens of seconds), we measure a bunching effect due to fluorescence intermittency that can not be described by fluctuations between two states with constant rates. The autocorrelation function also exhibits a non-stationary behavior related to power-law distributions of "On" and "Off" times.
Photons spontaneously emitted from single atoms are necessarily antibunched in time. The statistics of the photon time record, however, can show sub-Poissonian or even super-Poissonian statistics and depend strongly on the time interval used for analysis. In this work we have analyzed photon arrival times from resonantly excited barium atoms in an atomic beam observed under single-atom conditions. The time-interval dependence of photon statistics is presented, showing the connection between antibunching and sub-Poissonian statistics (at times comparable to the spontaneous-decay lifetime of the atom) as well as the evolution of the statistics in the long-time limit.