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.
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.
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).
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 photons are highly desirable for encoding, sending and processing quantum information. Suitable engineering of single quantum emitters and their environment can lead to a reliable single photon source and to mediated photon-photon interactions, essential assets for quantum communication and computation purposes. Dye molecules, our chosen single quantum emitter, have attracted much attention in recent years due to their high photostability and narrow emission lines. In this thesis I present a detailed analysis of the optical properties of single dibenzoterrylene molecules in an anthracene matrix. Single photon emission is demonstrated at room and cryogenic temperatures. In the latter case, an analysis of the second-order correlation function of the emission of a single molecule is studied at various temperatures. The data agree with a full solution of the optical Bloch equations over a wide range of temperature, and provide some insight into the dephasing process of the molecules. I then present a technique for integrating single dye molecules with nano-photonic devices. These are hybrid plasmonic waveguides, designed to guide light and to enhance the interaction with a single emitter by a tight confinement of the waveguide mode. Single molecules are deposited over the waveguides and a first evidence of coupling is presented. I conclude with proposed improvements to the optical setup and to the deposition methods. Finally, I present another type of integrated device, where the light matter interaction is enhanced by inserting single quantum emitters into coupled optical resonators. The theoretical description for the case of resonant two-photon absorption from single atoms in coupled photonic crystal cavities is developed. I conclude by proposing a possible realisation of this system, and describing the first steps towards the fabrication of such a device.
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.
Abstract Photonic quantum technology is essentially based on the exchange of individual photons as information carriers. Therefore, the development of practical single-photon sources that emit single photons on-demand is a crucial contribution to advance this emerging technology and to promote its first real-world applications. In the last two decades, a large number of quantum light sources based on solid-state emitters have been developed on a laboratory scale. Corresponding structures today have almost ideal optical and quantum-optical properties. For practical applications, however, one crucial factor is usually missing, namely direct on-chip fiber coupling, which is essential, for example, for the direct integration of such quantum devices into fiber-based quantum networks. In fact, the development of fiber-coupled quantum light sources is still in its infancy, with very promising advances having been made in recent years. Against this background, this review article presents the current status of the development of fiber-coupled quantum light sources based on solid-state quantum emitters and discusses challenges, technological solutions and future prospects. Among other things, the numerical optimization of the fiber coupling efficiency, coupling methods, and important realizations of such quantum devices are presented and compared. Overall, this article provides an important overview of the state-of-the-art and the performance parameters of fiber-coupled quantum light sources that have been achieved so far. It is aimed equally at experts in the scientific field and at students and newcomers who want to get an overview of the current developments.
High Resolution Image Download MS PowerPoint Slide Single photon sources are fundamental for applications in quantum computing, secure communication, and sensing, as they enable the generation of individual photons and ensure strict control over photon number statistics. However, current single photon sources can be limited by a lack of robustness, difficulty of integration into existing optical or electronic devices, and high cost. In this study, we present the use of off-the-shelf C 60 fullerene molecules embedded in polystyrene as room-temperature reliable single-photon emitters. As our results demonstrate, these molecules exhibit on-demand single-photon emission, with short fluorescence lifetimes and, consequently, high emission rates. The wide availability and ease of preparation and manipulation of fullerenes as single photon sources can pave the way for the development of practical, economic and scalable quantum photonic technologies.