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.
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.
Solid state quantum emitters are a mainstay of quantum nanophotonics as integrated single photon sources (SPS) and optical nanoprobes. Integrating such emitters with active nanophotonic elements is desirable in order to attain efficient control of their optical properties but typically degrades the photostability of the emitter itself. Here, we demonstrate a tuneable hybrid device that integrates lifetime-limited single emitters (linewidth ~ 40 MHz) and 2D materials at sub-wavelength separation without degradation of the emission properties. Our device's nanoscale dimensions enable ultra-broadband tuning (tuning range > 400 GHz) and fast modulation (frequency ~ 100 MHz) of the emission energy, which renders it an integrated, ultra-compact tuneable SPS. Conversely, this offers a novel approach to optical sensing of 2D material properties using a single emitter as a nanoprobe.Hybrid nanophotonic systems blend the strengths of distinct photonic elements to strongly enhance light-matter interactions 1 in integrated photonic circuits. In these systems, narrow-linewidth quantum light emitters play a key role as single photon sources (SPS) which interact with their nanoscale environment 2,3 . Controlling these interactions provides versatile SPS tuning 4 required for coupling quantum resources [5][6][7] . Integrating nanoscale light emitters with two-dimensional (2D) materials is motivated by the rich physics of near-field interactions 8 and new hybrid light-matter states 9,10 . This approach unites integrated solid-state SPS such as nitrogen vacancy centres 11 , quantum dots 12 and single molecules 13 with the diverse optoelectronic properties of 2D materials that facilitate emitting 14 , controlling [15][16][17] and detecting 18 light at the nanoscale. In such hybrid devices, quantum emitters can be integrated at sub-wavelength separation to the 2D interface to achieve efficient near-field coupling 8 , which modifies the emitter's radiative decay rate [19][20][21] or transition energy 22,23 . Recent experimental studies integrated 2D materials with ensembles of broadband emitters to demonstrate electrical 24-26 and electromechanical 27 tuning of the decay rate by controlling non-radiative energy transfer (nRET) or the energy flow to confined electromagnetic modes such as 2D polaritons 26,28 . Therefore, hybrids of 2D materials and SPS have the potential for in situ control of the conversion and channelling of single photons at the nanoscale. So far, these studies have been limited to ensembles and broad linewidth emitters. Integrating bright and narrow quantum emitters in such systems paves 2 the way towards a tuneable quantum light-matter interface, which is an essential ingredient for integrated quantum networks.Here, we demonstrate hybrid integration of 2D materials (semi-metallic graphene or semi-conducting MoS2) with single, lifetime-limited quantum emitters in nanocrystals to provide active emission control. Using the 2D materials as transparent electrodes, we show broadband Stark tuning of the emission energy o...
In this study we lay the groundwork for a graphene-based fundamental ruler at the nanoscale. It relies on the efficient energy-transfer mechanism between single quantum emitters and low-doped graphene monolayers. Our experiments, conducted with dibenzoterrylene (DBT) molecules, allow going beyond ensemble analysis due to the emitter photo-stability and brightness. A quantitative characterization of the fluorescence decayrate modification is presented and compared to a simple model, showing agreement with the − d 4 dependence, a genuine manifestation of a dipole interacting with a 2D material. With DBT molecules, we can estimate a potential uncertainty in position measurements as low as 5 nm in the range below 30 nm.
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.
Solid-state single photon sources (SPSs) with narrow linewidth play an important role in many leading quantum technologies. Within the wide range of SPSs studied to date, single fluorescent molecules hosted in organic crystals stand out as bright, photostable SPSs with lifetime-limited optical resonance at cryogenic temperatures. Furthermore, recent results have demonstrated that photostability and narrow linewidths are still observed from single molecules hosted in a nanocrystalline environment, which paves the way for their integration with photonic circuitry. Polymers offer a compatible matrix for embedding nanocrystals and provide a versatile yet low-cost approach for making nanophotonic structures on chip that guide light and enhance coupling to nanoscale emitters. Here, we present a deterministic nanostructuring technique based on electron-beam lithography for shaping polymers with embedded single molecules. Our approach provides a direct mean of structuring the nanoscale environment of narrow linewidth emitters while preserving their emission properties.Ideal SPSs are isolated quantum systems displaying stable emission within a narrow linewidth 1 , which is fundamental for quantum technology applications such as entanglement and single photon
The on-chip integration of quantum light sources and nonlinear elements poses a serious challenge to the development of a scalable photonic platform for quantum information and communication. In this work we demonstrate the potential of a novel hybrid technology which combines single organic molecules as quantum emitters and dielectric chips, consisting of ridge waveguides and grating far-field couplers. Dibenzoterrylene molecules in thin anthracene crystals exhibit long-term photostability, easy fabrication methods, almost unitary quantum yield and life-time limited emission at cryogenic temperatures. We couple such single emitters to silicon nitride ridge waveguide with a coupling efficiency of up to 42 ± 2 %, considering both propagation directions. The platform is devised to support both on-chip and free-space single photon processing.
We report on our recent progress in the study of single Dibenzoterrylene (DBT) molecules as single photon sources and nanoscale probes. We consider DBT molecules embedded in thin anthracene films, a system that allows stable single photon emission both at room and at cryogenic temperatures. We investigate the most important optical properties of the DBT:anthracene system as a whole. We then perform a full statistical study of the coupling between single DBT molecules by measuring the lifetimes of DBT both in the coupled and in the uncoupled case. The experimental results are framed into a simple universal scaling model, where the magnitude of coupling depends solely on universal parameters and on the distance d between the single emitter and the graphene monolayer. We apply this model to infer d and provide a proof of principle for a position ruler at the nanoscale [1].
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