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.
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.
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.
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.
Efficient quantum light sources and non-linear optical elements at the few photon level are the basic ingredients for most applications in nano and quantum technologies. On the other hand, a scalable platform for quantum ICT typically requires reliable light matter interfaces and on-chip integration. In this work we demonstrate the potential of a novel hybrid technology which combines single organic molecules as quantum emitters and dielectric chips [1]. Dibenzoterrylene molecules in anthracene crystals (DBT:Ac) are particularly suitable quantum systems for this task, since they exhibit long-term photostability in thin samples [2], easy fabrication methods and life-time limited emission at cryogenic temperatures [3]. We demonstrate at room temperature the emission of single photons from DBT molecules into ridge waveguides with a branching ratio up to 40%. The overall single-photon source efficiency, including emission into the guided mode, propagation losses, and emission into a quasi-gaussian mode in free space, is estimated around 16%. These results are competitive with state-of-the-art single photon emission into propagating guided modes from solid state systems [4], while offering a novel platform with unprecedented versatility. References [1] P. Lombardi et al., Arxiv: 1701.00459v1 (2017). [2] C. Toninelli et al., Opt. Express 18, 6577 (2010). [3] A. A. L. Nicolet et al., ChemPhysChem 8, 1929 (2007). [4] I. Zadeh et al., Nano Lett. 16, 2289 (2016); R. S. Daveau et al., Arxiv: 1610.08670v1 (2016). [5] J. Hwang et. al., New J. Phys. 13, 085009 (2011); H.-W. Lee et al., Phys. Rev. A 63, 012305 (2000).
Single organic molecules hold great promise for generating, manipulating, and storing single photons. Such processes form the basis for new quantum-enhanced technologies such as sensing, communications, and computation. In this talk I will focus on a particularly promising molecule – dibenzoterrylene (DBT). When DBT is introduced into a solid crystal of anthracene it is photostable and emits light between 780 and 795 nm. When cooled to cryogenic temperature, DBT is isolated from phonon-induced dephasing meaning that the photons have a lifetime-limited. I will present recent results in growing DBT-doped anthracene crystals, introducing these to nanophotonic interfaces for enhancing the collection of photons, tuning the DBT emission wavelength to coincide with rubidium atomic absorption, and finally pump-probe spectroscopy experiments to find long-lived triplet states in DBT which will be useful for building a single-molecule quantum memory.
The on-chip integration of quantum light sources and nonlinear elements constitutes a major step toward scalable photon-based quantum information processing and communication. In this work we demonstrate the potential of a hybrid technology that combines organic-molecule-based quantum emitters and dielectric chips consisting of ridge waveguides and grating far-field couplers. In particular, dibenzoterrylene molecules in thin anthracene crystals are used as single-photon sources, exhibiting long-term photostability, easy fabrication methods, almost unitary quantum yield, and lifetime-limited emission at cryogenic temperatures. We couple such single emitters to silicon nitride ridge waveguides, showing a coupling efficiency of up to 42 ± 2% over both propagation directions. Our results open a novel path toward a fully integrated and scalable photon-processing platform.
The development of single-photon sources has been nothing but rapid in recent years, with quantum emitter-based systems showing especially impressive progress. In this article, we give an overview of the developments in single-photon sources based on single molecules. We will introduce polycyclic hydrocarbons as the most commonly used emitter systems for the realization of an organic solid-state single-photon source. At cryogenic temperatures this special class of fluorescent molecules demonstrates remarkable optical properties such as negligible dephasing, indefinite photostability, and high photon rates, which make them attractive as fundamental building blocks in emerging quantum technologies. To better understand the general properties and limitations of these molecules, we discuss sample preparation and relevant emitter parameters such as absorption and emission spectra, lifetime, and dephasing. We will also give an overview of light extraction strategies as a crucial part of a single-photon source. Finally, we conclude with a look into the future, displaying current challenges and possible solutions.