Quantum technologies could largely benefit from the control of quantum emitters in sub-micrometric size crystals. These are naturally prone to integration in hybrid devices, including heterostructures and complex photonic devices. Currently available quantum emitters in nanocrystals suffer from spectral instability, preventing their use as single-photon sources for most quantum optics operations. In this work we report on the performances of single-photon emission from organic nanocrystals (average size of hundreds of nm), made of anthracene (Ac) and doped with dibenzoterrylene (DBT) molecules. The source has hours-long photostability with respect to frequency and intensity, both at room and at cryogenic temperature. When cooled to 3 K, the 00-zero phonon line shows linewidth values (50 MHz) close to the lifetime limit. Such optical properties in a nanocrystalline environment recommend the proposed organic nanocrystals as single-photon sources for integrated photonic quantum technologies.

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...

Single‐photon sources (SPSs) based on quantum emitters hold promise in quantum radiometry as metrology standard for photon fluxes at the low light level. Ideally this requires control over the photon flux in a wide dynamic range, sub‐Poissonian photon statistics, and narrow‐band emission spectrum. In this work, a monochromatic SPS based on an organic dye molecule is presented, whose photon flux is traceably measured to be adjustable between 144 000 and 1320 000 photons per second at a wavelength of (785.6 ± 0.1) nm, corresponding to an optical radiant flux between 36.5 and 334 fW. The high purity of the single‐photon stream is verified, with a second‐order autocorrelation function at zero time delay below 0.1 throughout the whole range. Such molecule‐based SPS is hence used for the calibration of a single‐photon avalanche detector against a low‐noise analog photodiode traceable to the primary standard for optical radiant flux (i.e., the cryogenic radiometer). Due to the narrow bandwidth of the source, corrections to the detector efficiency arising from the spectral power distribution are negligible. With this major advantage, the developed device may finally realize a low‐photon‐flux standard source for quantum radiometry.

The local interaction of charges and light in organic solids is the basis of distinct and fundamental effects. We here observe, at the single-molecule scale, how a focused laser beam can locally shift by hundreds of times their natural line width and, in a persistent way, the transition frequency of organic chromophores cooled at liquid helium temperature in different host matrices. Supported by quantum chemistry calculations, the results can be interpreted as effects of a photoionization cascade, leading to a stable electric field, which Stark-shifts the molecular electronic levels. The experimental observation is then applied to a common challenge in quantum photonics, i.e., the independent tuning and synchronization of close-by quantum emitters, which is desirable for multiphoton experiments. Five molecules that are spatially separated by about 50 μm and originally 20 GHz apart are brought into resonance within twice their line width. This tuning method, which does not require additional fabrication steps, is here independently applied to multiple emitters, with an emission line width that is only limited by the spontaneous decay and an inhomogeneous broadening limited to 1 nm. The system hence shows promise for photonic quantum technologies.

The successful development of future photonic quantum technologies will much depend on the possibility of realizing robust and scalable nanophotonic devices. These should include quantum emitters like on‐demand single‐photon sources and non‐linear elements, provided their transition linewidth is broadened only by spontaneous emission. However, conventional strategies to on‐chip integration, based on lithographic processes in semiconductors, are typically detrimental to the coherence properties of the emitter. Moreover, such approaches are difficult to scale and bear limitations in terms of geometries. Here an alternative platform is discussed, based on molecules that preserve near‐Fourier‐limited fluorescence even when embedded in polymeric photonic structures. 3D patterns are achieved via direct laser writing around selected molecular emitters, with a fast, inexpensive, and scalable fabrication process. By using an integrated polymeric design, detected photon counts of about 2.4 Mcps from a single cold molecule are reported. The proposed technology will allow for competitive organic quantum devices, including integrated multi‐photon interferometers, arrays of indistinguishable single‐photon sources, and hybrid electro‐optical nanophotonic chips.