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Journal of the Korean Physical Society

Statistical analysis of photons from a single terrylene molecule for the study of the energy level scheme

Kwang-Geol Lee

Published Jun 1, 2014• 4 citations
Publisher

Abstract

Single photons from single emitters are good candidates for a high-quality single-photon source which is essential in current quantum optical experiments and applications. Because the statistics of emitted photons is mainly determined by the energy level structure of the system, knowing the correct level scheme and the transition rates between levels is of primary importance. In this work, the energy level scheme and the photon-emission statistics of a single terrylene molecule are studied by measuring the second-order correlation function and the time trace of the emitted photons. The details in the measurement and analysis are discussed, and a more advanced energy-level structure of the terrylene molecule is suggested.

DOI
10.3938/jkps.64.1792

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Single photons from single emitters are good candidates for a high-quality single-photon source which is essential in current quantum optical experiments and applications. Because the statistics of emitted photons is mainly determined by the energy level structure of the system, knowing the correct level scheme and the transition rates between levels is of primary importance. In this work, the energy level scheme and the photon-emission statistics of a single terrylene molecule are studied by measuring the second-order correlation function and the time trace of the emitted photons. The details in the measurement and analysis are discussed, and a more advanced energy-level structure of the terrylene molecule is suggested.
Photons emitted from a single emitter are promising candidates for an efficient single-photon source, which is essential for many novel nano- and quantum-optical applications. As a photon source having a larger flux and high reliability is highly desirable. In this paper, we quantitatively studied the dependencies of the numbers of photons emitted and collected from single terrylene molecules on different experimental conditions, the refractive index of the substrate and the numerical aperture of the collection lens. Also, back-focal plane images are used to visualize the emission pattern of a single emitter.
Coherence length (time) is a key parameter in many classical and quantum optical applications. Two interferometers – Michelson and Young’s double-slit – are used to characterize the temporal coherence of single photons emitted from single terrylene molecules. For quantitative analysis, a dispersion-related distortion in the interference pattern of a Michelson interferometer is carefully corrected by a simple dispersion compensation. Additionally, it has been demonstrated that Young’s interferometer can be used in temporal coherence studies at the single photon level with high accuracy. The pros and cons of the two systems are discussed. The measured coherence lengths in the two systems are consistent with one another under the self-interference interpretations.
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.
Single molecules in suitable host crystals have been demonstrated to be useful single-photon emitters both at liquid-helium temperatures and at room temperature. The low-temperature source achieved controllable emission of single photons from a single terrylene molecule in p -terphenyl by an adiabatic rapid passage technique. In contrast with almost all other single-molecule systems, terrylene single molecules show extremely high photostability under continuous, high-intensity irradiation. A room-temperature source utilizing this material has been demonstrated, in which fast pumping into vibrational sidebands of the electronically excited state achieved efficient inversion of the emissive level. This source yielded a single-photon emission probability p (1) of 0.86 at a detected count rate near 300 000 photons s −1 , with very small probability of emission of more than one photon. Thus, single molecules in solids can be considered as contenders for applications of single-photon sources such as quantum key distribution.
Photon emission correlation spectroscopy is an indispensable tool for the study of atoms, molecules, and, more recently, solid-state quantum defects. In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology. Beyond an emitter's single-photon purity, however, photon correlation measurements can provide a wealth of information that can reveal details about its electronic structure and optical dynamics that are hidden by other spectroscopy techniques. This tutorial presents a standardized framework for using photon emission correlation spectroscopy to study quantum emitters, including discussion of theoretical background, considerations for data acquisition and statistical analysis, and interpretation. We highlight important nuances and best practices regarding the commonly-used g(2)(tau=0)<0.5g^{(2)}(\\tau=0)<0.5g(2)(tau=0)<0.5 test for single-photon emission. Finally, we illustrate how this experimental technique can be paired with optical dynamics simulations to formulate an electronic model for unknown quantum emitters, enabling the design of quantum control protocols and assessment of their suitability for quantum information science applications.