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Physical Review Letters

Photon antibunching in the fluorescence of a single dye molecule trapped in a solid

Th. Basché, W. E. Moerner, Michel Orrit, H. Talon

Published Sep 7, 1992• 578 citations
Publisher

Abstract

The correlation between fluorescence photons emitted by an optically pumped single molecule of pentacene in a p-terphenyl host has been investigated at short times. The correlation function shows photon antibunching, a unique feature of a nonclassical radiation field, which decreases if two molecules rather than one are pumped at the same time. The peculiarities of the correlation function for a three-level molecule are discussed and the theoretical description outlined.

DOI
10.1103/physrevlett.69.1516

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The correlation between fluorescence photons emitted by an optically pumped single molecule of pentacene in a p-terphenyl host has been investigated at short times. The correlation function shows photon antibunching, a unique feature of a nonclassical radiation field, which decreases if two molecules rather than one are pumped at the same time. The peculiarities of the correlation function for a three-level molecule are discussed and the theoretical description outlined.
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.
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.
The photon pair correlation in the laser-excited fluorescence of a single trapped and cooled Ba+{\mathrm{Ba}}^{+}Ba+ ion shows antibunching and, in addition, novel nonclassical phenomena absent in the fluorescence of two-level atoms. They include excessive transient values of the correlation caused by optical pumping, and temporally extended sub-Poissonian photon emission probability which arises from the transient excitation of nonabsorbing Raman coherence. The fluorescence also displays sub-Poissonian photon statistics.
Two-time correlations in the emissions of photons by a single atom of sodium in the presence of a coherent exciting field near resonance have been investigated. In the experiment sodium atoms in an atomic beam are excited by a perpendicular light beam from a tunable dye laser, and they are prepared by optical pumping to behave as two-level quantum systems. The fluorescent light is collected by a microscope objective in a direction that is approximately orthogonal to both beams and imaged on two photomultipliers. Photoelectric pulse correlations are measured in the presence of exciting fields of various strengths and for various detunings from the atomic resonance, and are found to exhibit significant nonclassical features. The results show clearly that the emitted photons exhibit antibunching, in good quantitative agreement with the predictions of quantum electrodynamics.
Photon antibunching in resonance fluorescence - the emission from a single, resonantly driven two-level quantum emitter - is a paradigmatic signature of nonclassical light. Photon entanglement, by contrast, manifests as correlations that can defy any classical description and is typically regarded as a distinct quantum effect. Here, we experimentally extract pairs of narrowband, time-bin-entangled photons from the antibunched resonance fluorescence of a single trapped atom. We verify entanglement via violation of the CHSH Bell inequality and by reconstructing the two-photon density matrix. The observed correlations vanish when the coincidence time window exceeds the antibunching timescale, revealing underlying multimode entanglement in the emitted field. Our results establish a direct link between photon antibunching and photon-photon entanglement, unifying two canonical signatures of nonclassical light.
We used scanning confocal microscopy to study the fluorescence from a single terrylene molecule embedded in a thin polymer film of polymethyl methacrylate, at room temperature, with a high signal-to-background ratio. The photon-pair correlation function g((2))(tau) exhibits perfect photon antibunching at tau = 0 and a limit of 1.3, compatible with bunching associated with the molecular triplet state. Application of this molecular system to a triggered single-photon source based on single-molecule fluorescence is investigated.