Isolating single molecules in the solid state has allowed fundamental experiments in basic and applied sciences. When cooled down to liquid helium temperature, certain molecules show transition lines, that are tens of megahertz wide, limited only by the excited state lifetime. The extreme flexibility in the synthesis of organic materials provides, at low costs, a wide palette of emission wavelengths and supporting matrices for such single chromophores. In the last decades, the controlled coupling to photonic structures has led to an optimized interaction efficiency with light. Molecules can hence be operated as single photon sources and as non-linear elements with competitive performance in terms of coherence, scalability and compatibility with diverse integrated platforms. Moreover, they can be used as transducers for the optical read-out of fields and material properties, with the promise of single-quanta resolution in the sensing of charges and motion. We show that quantum emitters based on single molecules hold promise to play a key role in the development of quantum science and technologies.Modern societies have an ever-growing need for efficient computation techniques and for fast and secure communication, to distribute a huge amount of data around the globe. By harnessing quantum effects present at the nanoscale, new quantum technologies can be employed to meet these needs, including quantum cryptography and fully-fledged quantum information processing. On the other hand, the extreme sensitivity of quantum systems to their local environment can be exploited to also create new sensing devices, which provide unprecedented precision, accuracy and resolution and can be deployed within large quantum networks. Key applications require the generation and manipulation of quantum states of light, such as photonic quantum simulation [1, 2], linear optical quantum computing [3], device-independent or long-distance quantum key distribution protocols [4], sub-shot-noise imaging [5] and quantum metrology [6,7]. In this context, single impurities in solid-state systems can act as bright, on-demand single-photon sources (SPSs), which are a crucial resource in these photonic quantum technologies. Quantum emitters may also perform as non-linear elements at the few-photon level [8] and as nanoscale sensors, allowing the optical read-out of local properties of materials and fields. In this context, single molecules in the solid-state offer competitive and reliable properties, with several key advantages. First, they are very small and have well-defined transition dipole moments so that they can be used as nanoscopic sensors for a number of scalar and vector quantities such as pressure, strain, temperature, electric and magnetic fields, as well as optical fields. Second, organic molecules can be designed and synthesized for different parts of the visible spectrum and integrated in a range of organic matrices, a feature that is a severe limiting factor for color centers in diamond or lithographically produced semiconductor quan...

Organic molecules have recently gained attention as novel sources of single photons. We present a joint experiment-theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single molecule. We observe spectra with a zero-phonon-line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localised vibrational modes of the molecule and a thermal phonon bath, which we include non-perturbatively, and is able capture all observed features. For resonant driving we measure Rabi oscillations that become increasingly damped with temperature, which our model naturally reproduces. Our results constitute an essential characterisation of the photon coherence of these promising molecules, paving the way towards their use in future quantum information applications.

Single dibenzoterrylene (DBT) molecules offer great promise as bright, reliable sources of single photons on demand, capable of integration into solid-state devices. It has been proposed that DBT in anthracene might be placed close to an optical waveguide for this purpose, but so far there have been no demonstrations of sufficiently thin crystals, with a controlled concentration of the dopant molecules. Here we present a method for growing very thin anthracene crystals from super-saturated vapour, which produces crystals of extreme flatness and controlled thickness. We show how this crystal can be doped with an adjustable concentration of dibenzoterrylene (DBT) molecules and we examine the optical properties of these molecules to demonstrate their suitability as quantum emitters in nanophotonic devices. Our measurements show that the molecules are available in the crystal as single quantum emitters, with a well-defined polarisation relative to the crystal axes, making them amenable to alignment with optical nanostructures. We find that the radiative lifetime and saturation intensity vary little within the crystal and are not in any way compromised by the unusual matrix environment. We show that a large fraction of these emitters can be excited more than 10 times without photo-bleaching, making them suitable for real applications.

The longitudinal (?????) and transverse (?????) decay rates of a two-level quantum system have profound influence on its evolution. Atomic systems with ?????=??????? have been studied extensively, but with the rise of solid-state quantum devices it is also important to consider the effect of stronger transverse relaxation due to interactions with the solid environment. Here we study the quantum dynamics of a single organic dye molecule driven by a laser. We measure the variation of ????? with temperature and determine the activation energy for thermal dephasing of the optical dipole. Then we measure the second-order correlation function g????????(??) of the light emitted by the molecule for various ratios ?????/????? and saturation parameters S. We show that the general solution to the optical Bloch equations accurately describes the observed quantum dynamics over a wide range of these parameters, and we discuss the limitations of the various approximate expressions for g????????(??) that appear in the literature

Dibenzoterrylene (DBT) molecules within a crystalline anthracene matrix show promise as quantum emitters for controlled, single photon production. We present the design and construction of a chamber in which we reproducibly grow doped anthracene crystals of optical quality that are several mm across and a few μm thick. We demonstrate control of the DBT concentration over the range 6–300 parts per trillion and show that these DBT molecules are stable single-photon emitters. We interpret our data with a simple model that provides some information on the vapour pressure of DBT.

We demonstrate the emission of photons from a single molecule into a hybrid gap plasmon waveguide (HGPW). Crystals of anthracene, doped with dibenzoterrylene (DBT), are grown on top of the waveguides. We investigate a single DBT molecule coupled to the plasmonic region of one of the guides, and determine its in-plane orientation, excited state lifetime and saturation intensity. The molecule emits light into the guide, which is remotely out-coupled by a grating. The second-order autocorrelation and cross-correlation functions show that the emitter is a single molecule and that the light emerging from the grating comes from that molecule. The coupling efficiency is found to be β W G = 11.6(1.5)%. This type of structure is promising for building new functionality into quantum-photonic circuits, where localised regions of strong emitter-guide coupling can be interconnected by low-loss dielectric guides.

A reliable single photon source is required for many aspects of quantum technology. Organic molecules are attractive for this application because they can have high quantum yield and can be photostable, even at room temperature. To generate a photon with high probability, a laser must excite the molecule efficiently. We develop a simple model for that efficiency and discuss how to optimise it. We demonstrate the validity of our model through experiments on a single dibenzoterrylene (DBT) molecule in an anthracene crystal. We show that the excitation probability cannot exceed 75% at room temperature, but can increase to over 99% if the sample is cooled to liquid nitrogen temperature. The possibility of high photon generation efficiency with only modest cooling is a significant step towards a reliable photon source that is simple and practical.

Extinction spectroscopy is a powerful tool for demonstrating the coupling of a single quantum emitter to a photonic structure. However, it can be challenging in all but the simplest of geometries to deduce an accurate value of the coupling efficiency from the measured spectrum. Here we develop a theoretical framework to deduce the coupling efficiency from the measured transmission and reflection spectra without precise knowledge of the photonic environment. We then consider the case of a waveguide interrupted by a transverse cut in which an emitter is placed. We apply that theory to a silicon nitride waveguide interrupted by a gap filled with anthracene that is doped with dibenzoterrylene molecules. We describe the fabrication of these devices, and experimentally characterise the waveguide coupling of a single molecule in the gap.