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arXiv:1011.6153 · Optics Express

Efficient generation of near infra-red single photons from the zero-phonon line of a single molecule

Jean-Baptiste Trebbia, H. Ruf, Philippe Tamarat, Brahim Lounis

Published Dec 16, 2009• 51 citations
arXivHTMLPDF

Abstract

Using the zero-phonon line (ZPL) emission of a single molecule, we realized a triggered source of near-infra-red (lambda = 785 nm) single photons at a high repetition rate. A Weierstrass solid immersion lens is used to image single molecules with an optical resolution of 300 nm (approximately 0.4lambda) and a high collection efficiency. Because dephasing of the transition dipole due to phonons vanishes at liquid helium temperatures, our source is attractive for the efficient generation of single indistinguishable photons.

DOI
10.1364/oe.17.023986

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Using the zero-phonon line (ZPL) emission of a single molecule, we realized a triggered source of near-infra-red (lambda = 785 nm) single photons at a high repetition rate. A Weierstrass solid immersion lens is used to image single molecules with an optical resolution of 300 nm (approximately 0.4lambda) and a high collection efficiency. Because dephasing of the transition dipole due to phonons vanishes at liquid helium temperatures, our source is attractive for the efficient generation of single indistinguishable photons.
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By using the zero-phonon line emission of an individual organic molecule, we realized a source of indistinguishable single photons in the near infrared. A Hong-Ou-Mandel interference experiment is performed and a two-photon coalescence probability higher than 5050%50 at 2 K is obtained. The contribution of the temperature-dependent dephasing processes to the two-photon interference contrast is studied. We show that the molecule delivers nearly ideal indistinguishable single photons at the lowest temperatures when the dephasing is nearly lifetime limited. This source is used to generate postselected polarization-entangled photon pairs as a test bench for applications in quantum information.
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.
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.
Single photons are very attractive for quantum information processing, given their long coherence time and their ability to carry information in many degrees of freedom. A current challenge is the generation of single photons in a photonic chip in order to scale up the complexity of quantum operations. Solid state emitters could offer this possibility. Quantum dots are one promising approach, but photons produced by different dots are generally distinguishable. Nitrogen-vacancy (N-V) centres in diamond are also promising, however it is challenging to place these in photonic circuits and the emitted photons have many frequencies. By contrast, dibenzoterrylene (DBT) molecules embedded in a thin film of anthracene (AC) at cryogenic temperatures produce a high yield of indistinguishable photons [1, 2]. DBT acts as a two-level system with a narrow 30 MHz near-infrared (785 nm) zero-phonon line [1]. We have proposed that a DBT molecule, deposited in the vicinity of a nanoscale waveguide, could emit these photons efficiently into the waveguide [3]. Conventional spin-coating methods [1] do not offer sufficient control over the surface coverage and the morphology of the AC crystal for deposition on photonic structures, while crystals grown with sublimation are too thick. Another method is needed.
Single molecules of polyaromatic hydrocarbons (PAH) in suitable host matrices are known for emitting with high quantum efficiency in very narrow and stable zero-phonon lines (ZPL) [1]. For our experiments we used dibenzotherrylene (DBT) molecule inserted as impurity in anthracene (Ac) nanocrystals, dispersed on a gold substrate and cooled down to 3 K in a closed-cycle cryostat. DBT in Ac features a single-photon dipole-allowed transition around 784 nm. Each molecule is namely identical but environmental conditions like local trapped charges or crystal strain can shift the frequency of its transition in a range of approximately 1 nm [2]. Those static differences alongside any instantaneous interaction with the environment can degrade the ability of the emitted photons to undergo two-photon interference (TPI).