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Physica Scripta

Emission Properties of a Single Photon Source

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

Published Jan 1, 2004• 4 citations
Publisher

Abstract

We report on the realization of a single photon source relying on the pulsed excitation of a single organic molecule at room temperature, and the study of its intensity fluctuations over 4 orders of magnitude of the observation time scale. On a time scale of a few excitation periods, sub-poissonian statistics is clearly observed and the probability of multiphoton events is 10 times smaller than for equivalent Poissonian pulses. An excess of noise appears on longer timescale, due to the blinking produced by the molecular triplet state.

DOI
10.1238/physica.topical.112a00095

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We report on the realization of a single photon source relying on the pulsed excitation of a single organic molecule at room temperature, and the study of its intensity fluctuations over 4 orders of magnitude of the observation time scale. On a time scale of a few excitation periods, sub-poissonian statistics is clearly observed and the probability of multiphoton events is 10 times smaller than for equivalent Poissonian pulses. An excess of noise appears on longer timescale, due to the blinking produced by the molecular triplet state.
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.
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 generation of non-classical states of light [1] is an important scientific challenge with many potential applications. For example, squeezed states of light [2] have generated much interest in the past decade, because measurements can be performed with noise levels that are lower than those available with classical light. A particularly novel non-classical source of light is a triggered single-photon source: a source that has the property to emit with a high degree of certainty one (and only one) photon at a user-specified time. Such a deterministic source of single photons can be important for quantum information processing [3], quantum cryptography [4] and certain quantum computation problems [5]. A single quantum emitter such as a molecule or an atom is a good potential source because it can emit only one photon at a time. The emitted light is antibunched [6, 7] and consists of single photons separated by random time intervals, which depend on the excited state lifetime and on the pumping rate. Thus triggered emission of single photons can be obtained with controlled excitation of a single emitter. The first demonstration of a single photons source [8] using a single molecule in a solid is based on a rapid adiabatic passage method [9] to excite the molecule. In the effective spin picture, the Bloch vector follows the driving magnetic field adiabatically if the laser-molecule frequency detuning is swept slowly through the resonance. Since the passage inverts the field, the system goes from the ground to the excited state. From this fluorescent state the molecule can emit only a single photon. The molecular resonance is swept by Stark effect at fixed laser frequency. This is done easily by applying a radio frequency electric field to the molecule. The results showed photon states with statistics that differ radically from those of coherent states. But this method requires cryogenic temperatures (2K) since narrow zero phonon lines are needed for the adiabatic following. At room temperature a source of triggered single photons based on the concept of pulsed optical excitation of a single highly fluorescent molecule has been demonstrated [10]. A short pulse of green laser light pumps the molecule from the ground state to a vibronically excited level of the first electronic excited state. After fast (ps) relaxation to the lowest electronic excited state, the molecule subsequently emits a single photon. A frequency-doubled mode-locked Nd-YAG laser is used to pump highly stable single terrylene molecules contained in a p-terphenyl molecular crystal where they are protected from exposure to diffusing quenchers (such as oxygen). The result shows that the photons are emitted after the laser pulses at times separated by the laser repetition time within the lifetime of terrylene in p-terphenyl. Since the pump pulse width is very short compared to the fluorescence lifetime, the probability of two (or more) photon emission per pulse is always zero. At the maximum laser power, 90% of the laser pulses lead to a single photon emission. The parameters of this source (repetition rate and single photon generation probability) were limited only by the laser system used; nevertheless, this performance already surpasses that of previous work. The high performance combined with the vanishing two photon emission probability and the simplicity of this source suggests that it can be considered for a variety of quantum optical experiments and for secure quantum cryptography [11]. Semiconductor quantum dots (QD) are other potential systems for single photon generation [12]. QDs are often referred to as “artificial atoms” because many of their optical properties, such as ultranarrow transitions, arise from discrete, atomic-like energy levels [13, 14]. To reinforce this analogy a study of the photon antibunching in this system was needed. QDs differ from atoms and molecules since the creation of multiple excitons is possible in QDs. Consequently, if two electron-hole pairs can radiatively recombine, the simultaneous emission of two photons from a QD is then possible. Thus different regimes of photon statistics were expected because the probability of multiple exciton creation depends on excitation intensity. The fluorescence intensity correlation function of a single CdSe quantum dot has been investigated [15] using a coincidence setup (start-stop experiment). A strong photon antibunching has been observed over a large range of intensities (0.1-100 kW/cm2). The lack of coincidence at zero time delay indicates a highly efficient Auger ionization process [16], which suppresses multi-photon emission in these colloidal quantum dots. This result shows that room temperature single photon sources can be achieved with colloidal nanoparticles.
We investigate the photon statistics of a single-photon source that operates under non-stationary conditions. The photons are emitted by shining a periodic sequence of laser pulses on single atoms falling randomly through a high-finesse optical cavity. Strong antibunching is found in the intensity correlation of the emitted light, demonstrating that a single atom emits photons one at a time. However, the number of atoms interacting with the cavity follows a Poissonian statistics so that, on average, no sub-Poissonian photon statistics is obtained, unless the measurement is conditioned on the presence of single atoms.
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.
Abstract Since the onset of the 1990s, the development of single-molecule spectroscopy has led to the discovery of various quantum optical signatures in organic single molecules. The single-photon nature of an organic chromophore is of particular importance because of its potential as a nonclassical photon source at room temperature for quantum information science and optical quantum computing. This condensed review focuses on the introduction of fundamental knowledge and basic experimental methods for single-photon sources and organic molecular photophysics and summarizes the research developments in this field, providing an understanding of quantum emission from organic single molecules.