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arXiv:0810.4258 · Journal of Modern Optics

Molecules as sources for indistinguishable single photons

Ville Ahtee, R. Lettow, R. Pfab, Alois Renn, Erkki Ikonen, Stephan Götzinger, Vahid Sandoghdar

Published Jan 16, 2009• 18 citations
arXivHTMLPDF

Abstract

We report on the triggered generation of identical photons by solid-state single-photon sources in two separate cryogenic laser scanning microscopes. Organic fluorescent molecules were used as emitters and investigated by means of high resolution laser spectroscopy. Continuous-wave photon correlation measurements on individual molecules proved the isolation of single quantum systems. By using frequency selective pulsed excitation of the molecule and efficient spectral filtering of its emission, we produced triggered Fourier-limited single photons. In a further step, local electric fields were applied to match the emission wavelengths of two different molecules via Stark effect. Identical single photons are indispensable for the realization of various quantum information processing schemes proposed. The solid-state approach presented here paves the way to the integration of multiple bright sources of single photons on a single chip.

DOI
10.1080/09500340802464657

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We report on the triggered generation of identical photons by solid-state single-photon sources in two separate cryogenic laser scanning microscopes. Organic fluorescent molecules were used as emitters and investigated by means of high resolution laser spectroscopy. Continuous-wave photon correlation measurements on individual molecules proved the isolation of single quantum systems. By using frequency selective pulsed excitation of the molecule and efficient spectral filtering of its emission, we produced triggered Fourier-limited single photons. In a further step, local electric fields were applied to match the emission wavelengths of two different molecules via Stark effect. Identical single photons are indispensable for the realization of various quantum information processing schemes proposed. The solid-state approach presented here paves the way to the integration of multiple bright sources of single photons on a single chip.
We demonstrate two solid-state sources of indistinguishable single photons. High resolution laser spectroscopy and optical microscopy were combined at T = 1.4 K to identify individual molecules in two independent microscopes. The Stark effect was exploited to shift the transition frequency of a given molecule and thus obtain single photon sources with perfect spectral overlap. Our experimental arrangement sets the ground for the realization of various quantum interference and information processing experiments.
We demonstrate two solid-state sources of indistinguishable single photons. High resolution laser spectroscopy and optical microscopy were combined at T = 1.4 K to identify individual molecules in two independent microscopes. The Stark effect was exploited to shift the transition frequency of a given molecule and thus obtain single photon sources with perfect spectral overlap. Our experimental arrangement sets the ground for the realization of various quantum interference and information processing experiments. (c) 2007 Optical Society of America.
Single molecules in solid state matrices have been proposed as sources of single photon Fock states back 20 years ago. Their success in quantum optics and in many other research fields stems from the simple recipes used in the preparation of samples, with hundreds of nominally identical and isolated molecules. Main challenges as of today for their application in photonic quantum technologies are the optimization of light extraction and the on-demand emission of indistinguishable photons. We here present Hong–Ou–Mandel (HOM) experiments with photons emitted by a single molecule of dibenzoterrylene in an anthracene nanocrystal at 3 K, under continuous wave and also pulsed excitation. A detailed theoretical model is applied, which relies on independent measurements for most experimental parameters, hence allowing for an analysis of the different contributions to the two-photon interference visibility, from residual dephasing to spectral filtering. A HOM interference visibility of more than 75% is reported, which, according to the model, is limited by the residual dephasing present at the operating temperature.
Quantum light sources are crucial for the future of quantum photonic technologies and, among them, single photons on-demand are key resources in quantum communications and information processing. Ideal quantum emitters providing indistinguishable photons in a clocked manner, negligible decoherence and spectral diffusion, and with potential for scalability are today still a major challenge. We report on photostable and indistinguishable single photon emission from dibenzoterrylene molecules isolated in anthracene nanocrystals (DBT:Ac NCs) at 3K. The visibility of two-photon interference is preserved even when they are separated more than thirty times the excited-state lifetime, or ten fluorescence cycles. One of the advantages of organic molecules is the low-cost mass production of nominally identical emitters, that also allow for on-chip integration. These aspects combined with high spectral stability and coherence make them promising for applications and future quantum technologies.
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 molecules in solid-state matrices have been proposed as sources of single-photon Fock states back 20 years ago. Their success in quantum optics and in many other research fields stems from the simple recipes used in the preparation of samples, with hundreds of nominally identical and isolated molecules. Main challenges as of today for their application in photonic quantum technologies are the optimization of light extraction and the on-demand emission of indistinguishable photons. We here present Hong-Ou-Mandel experiments with photons emitted by a single molecule of dibenzoterrylene in an anthracene nanocrystal at 3 K, under continuous wave and also pulsed excitation. A detailed theoretical model is applied, which relies on independent measurements for most experimental parameters, hence allowing for an analysis of the different contributions to the two-photon interference visibility, from residual dephasing to spectral filtering.