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Solid-state spin-photon interfaces that combine single-photon generation and long-lived spin coherence with scalable device integration-ideally under ambient conditions-hold great promise for the implementation of quantum networks and sensors. Despite rapid progress reported across several candidate systems, those possessing quantum coherent single spins at room temperature remain extremely rare. Here we report quantum coherent control under ambient conditions of a single-photon-emitting defect spin in a layered van der Waals material, namely, hexagonal boron nitride. We identify that the carbon-related defect has a spin-triplet electronic ground-state manifold. We demonstrate that the spin coherence is predominantly governed by coupling to only a few proximal nuclei and is prolonged by decoupling protocols. Our results serve to introduce a new platform to realize a room-temperature spin qubit coupled to a multiqubit quantum register or quantum sensor with nanoscale sample proximity.
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Negatively charged boron vacancies (VB-) in hexagonal boron nitride (hBN) have recently gained interest as spin defects for quantum information processing and quantum sensing by a layered material. However, the boron vacancy can exist in a number of charge states in the hBN lattice, but only the -1 state has spin-dependent photoluminescence and acts as a spin-photon interface. Here, we investigate the charge state switching of VB defects under laser and electron beam excitation. We demonstrate deterministic, reversible switching between the -1 and 0 states (VB- â VB0 + e-), occurring at rates controlled by excess electrons or holes injected into hBN by a layered heterostructure device. Our work provides a means to monitor and manipulate the VB charge state, and to stabilize the -1 state which is a prerequisite for spin manipulation and optical readout of the defect.
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Light-matter interactions in optical cavities underpin many applications of integrated quantum photonics. Among various solid-state platforms, hexagonal boron nitride (hBN) is gaining considerable interest as a compelling van der Waals host of quantum emitters. However, progress to date has been limited by an inability to engineer simultaneously an hBN emitter and a narrow-band photonic resonator at a predetermined wavelength. Here, we overcome this problem and demonstrate deterministic fabrication of hBN nanobeam photonic crystal cavities with high quality factors over a broad spectral range (â¼400 to 850 nm). We then fabricate a monolithic, coupled cavity-emitter system designed for a blue quantum emitter that has an emission wavelength of 436 nm and is induced deterministically by electron beam irradiation of the cavity hotspot. Our work constitutes a promising path to scalable on-chip quantum photonics and paves the way to quantum networks based on van der Waals materials.
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Strong coupling (SC) between light and matter excitations bears intriguing potential for manipulating material properties. Typically, SC has been achieved between mid-infrared (mid-IR) light and molecular vibrations or between visible light and excitons. However, simultaneously achieving SC in both frequency bands remains unexplored. Here, we introduce polaritonic nanoresonators (formed by h-BN layers on Al ribbons) hosting surface plasmon polaritons (SPPs) at visible frequencies and phonon polaritons (PhPs) at mid-IR frequencies, which simultaneously couple to excitons and molecular vibrations in an adjacent layer of CoPc molecules, respectively. Employing near-field optical nanoscopy, we demonstrate the colocalization of near fields at both visible and mid-IR frequencies. Far-field transmission spectroscopy of the nanoresonator structure covered with a layer of CoPc molecules shows clear mode splittings in both frequency ranges, revealing simultaneous SPP-exciton and PhP-vibron coupling. Dual-band SC may offer potential for manipulating coupling between exciton and molecular vibration in future optoelectronics, nanophotonics, and quantum information applications.
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The time-dependent Mandel Q parameter, Q(T), provides a measure of photon number variance for a light source as a function of integration time. Here, we use Q(T) to characterise single photon emission from a quantum emitter in hexagonal boron nitride (hBN). Under pulsed excitation a negative Q parameter was measured, indicating photon antibunching at an integration time of 100â ns. For larger integration times Q is positive and the photon statistics become super-Poissonian, and we show by comparison with a Monte Carlo simulation for a three-level emitter that this is consistent with the effect of a metastable shelving state. Looking towards technological applications for hBN single photon sources, we propose that Q(T) provides valuable information on the intensity stability of single photon emission. This is useful in addition to the commonly used g(2)(τ) function for the complete characterisation of a hBN emitter.
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Hexagonal boron nitride (hBN) has emerged as a fascinating platform to explore quantum emitters and their applications. Beyond being a wide-bandgap material, it is also a van der Waals crystal, enabling direct exfoliation of atomically thin layersâa combination which offers unique advantages over bulk, 3D crystals. In this Mini Review we discuss the unique properties of hBN quantum emitters and highlight progress toward their future implementation in practical devices. We focus on engineering and integration of the emitters with scalable photonic resonators. We also highlight recently discovered spin defects in hBN and discuss their potential utility for quantum sensing. All in all, hBN has become a front runner in explorations of solid-state quantum science with promising future prospects.
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Resonance fluorescence from a quantum emitter is an ideal source to extract indistinguishable photons. By using the cross-polarization to suppress the laser scattering, we observed resonance fluorescence from GeV color centers in diamond at cryogenic temperature. The Fourier-transform-limited line width emission with T2/2T1 â¼ 0.86 allows for two-photon interference based on single GeV color center. Under pulsed excitation, the separated photons exhibit a Hong-Ou-Mandel quantum interference above classical limit, whereas the continuous-wave excitation leads to a coalescence time window of 1.05 radiative lifetime. In addition, we demonstrated a single-shot readout of spin states with a fidelity of 74%. Our experiments lay down the foundation for building a quantum network with GeV color centers in diamond.
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Coherent coupling of defect spins with surrounding nuclei along with the endowment to read out the latter are basic requirements for an application in quantum technologies. We show that negatively charged boron vacancies (VB-) in hexagonal boron nitride (hBN) meet these prerequisites. We demonstrate Hahn-echo coherence of the VB- spin with a characteristic decay time Tcoh = 15 µs, close to the theoretically predicted limit of 18 µs for defects in hBN. Elongation of the coherence time up to 36 µs is demonstrated by means of the Carr-Purcell-Meiboom-Gill decoupling technique. Modulation of the Hahn-echo decay is shown to be induced by coherent coupling of the VB- spin with the three nearest 14N nuclei via a nuclear quadrupole interaction of 2.11 MHz. DFT calculation confirms that the electron-nuclear coupling is confined to the defective layer and stays almost unchanged with a transition from the bulk to the single layer.
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Quantum emitters are needed for a myriad of applications ranging from quantum sensing to quantum computing. Hexagonal boron nitride (hBN) quantum emitters are one of the most promising solid-state platforms to date due to their high brightness and stability and the possibility of a spin-photon interface. However, the understanding of the physical origins of the single-photon emitters (SPEs) is still limited. Here we report dense SPEs in hBN across the entire visible spectrum and present evidence that most of these SPEs can be well explained by donor-acceptor pairs (DAPs). On the basis of the DAP transition generation mechanism, we calculated their wavelength fingerprint, matching well with the experimentally observed photoluminescence spectrum. Our work serves as a step forward for the physical understanding of SPEs in hBN and their applications in quantum technologies.
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Integration of solid-state quantum emitters into nanophotonic circuits is a critical step towards fully on-chip quantum photonic-based technologies. Among potential materials platforms, quantum emitters in hexagonal boron nitride (hBN) have emerged as a viable candidate over the last years. While the fundamental physical properties have been intensively studied, only a few works have focused on the emitter integration into photonic resonators. Yet, for a potential quantum photonic material platform, the integration with nanophotonic cavities is an important cornerstone, as it enables the deliberate tuning of the spontaneous emission and the improved readout of distinct transitions for a quantum emitter. In this work, the resonant tuning of a monolithic cavity integrated hBN quantum emitter is demonstrated through gas condensation at cryogenic temperature. In resonance, an emission enhancement and lifetime reduction are observed, with an estimate for the Purcell factor of ≈15.
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Single-photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered increasing attention over the last few years due to their superior optical properties. However, despite the vast range of experimental results and theoretical calculations, the defect structure responsible for the observed emission has remained elusive. Here, by controlling the incorporation of impurities into hBN via various bottom-up synthesis methods and directly through ion implantation, we provide direct evidence that the visible SPEs are carbon related. Room-temperature optically detected magnetic resonance is demonstrated on ensembles of these defects. We perform ion-implantation experiments and confirm that only carbon implantation creates SPEs in the visible spectral range. Computational analysis of the simplest 12 carbon-containing defect species suggest the negatively charged [Formula: see text] defect as a viable candidate and predict that out-of-plane deformations make the defect environmentally sensitive. Our results resolve a long-standing debate about the origin of single emitters at the visible range in hBN and will be key to the deterministic engineering of these defects for quantum photonic devices.
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This publisher's note contains a correction to Opt. Lett.47, 1673 (2022)10.1364/OL.454450.
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High-purity single-photon sources (SPS) that can operate at room temperature are highly desirable for a myriad of applications, including quantum photonics and quantum key distribution. In this work, we realize an ultra-bright solid-state SPS based on an atomic defect in hexagonal boron nitride (hBN) integrated with a solid immersion lens (SIL). The SIL increases the source efficiency by a factor of six, and the integrated system is capable of producing over ten million single photons per second at room temperature. Our results are promising for practical applications of SPS in quantum communication protocols.
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Negatively charged boron vacancy (V_{B}^{-}) centers in hexagonal boron nitride (h-BN) are promising spin defects in a van der Waals crystal. Understanding the spin properties of the excited state (ES) is critical for realizing dynamic nuclear polarization. Here, we report zero-field splitting in the ES of D_{ES}=2160 MHz and its associated optically detected magnetic resonance (ODMR) contrast of 12% at cryogenic temperature. In contrast to nitrogen vacancy (NV^{-}) centers in diamond, the ODMR contrast of V_{B}^{-} centers is more prominent at cryotemperature than at room temperature. The ES has a g factor similar to the ground state. The ES photodynamics is further elucidated by measuring the level anticrossing of the V_{B}^{-} defects under varying external magnetic fields. Our results provide important information for utilizing the spin defects of h-BN in quantum technology.
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Energy and charge transfer processes in interacting donor-acceptor systems are the bedrock of many fundamental studies and technological applications ranging from biosensing to energy storage and quantum optoelectronics. Central to the understanding and utilization of these transfer processes is having full control over the donor-acceptor distance. With their atomic thickness and ease of integrability, two-dimensional materials are naturally emerging as an ideal platform for the task. Here, we review how van der Waals semiconductors are shaping the field. We present a selection of some of the most significant demonstrations involving transfer processes in layered materials that deepen our understanding of transfer dynamics and are leading to intriguing practical realizations. Alongside current achievements, we discuss outstanding challenges and future opportunities.
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We demonstrate the fabrication of large-scale arrays of single-photon emitters (SPEs) in hexagonal boron nitride (hBN). Bottom-up growth of hBN onto nanoscale arrays of dielectric pillars yields corresponding arrays of hBN emitters at the pillar sites. Statistical analysis shows that the pillar diameter is critical for isolating single defects, and diameters of â¼250 nm produce a near-unity yield of a single emitter at each pillar site. Our results constitute a promising route toward spatially controlled generation of hBN SPEs and provide an effective and efficient method to create large-scale SPE arrays. The results pave the way to scalability and high throughput fabrication of SPEs for advanced quantum photonic applications.
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Color centers in hexagonal boron nitride (hBN) are becoming an increasingly important building block for quantum photonic applications. Herein, we demonstrate the efficient coupling of recently discovered spin defects in hBN to purposely designed bullseye cavities. We show that boron vacancy spin defects couple to the monolithic hBN cavity system and exhibit a 6.5-fold enhancement. In addition, by comparative finite-difference time-domain modeling, we shed light on the emission dipole orientation, which has not been experimentally demonstrated at this point. Beyond that, the coupled spin system exhibits an enhanced contrast in optically detected magnetic resonance readout and improved signal-to-noise ratio. Thus, our experimental results, supported by simulations, constitute a first step toward integration of hBN spin defects with photonic resonators for a scalable spin-photon interface.
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Fluorescent nanoparticles are widely utilized in a large range of nanoscale imaging and sensing applications. While ultra-small nanoparticles (size ≤10 nm) are highly desirable, at this size range, their photostability can be compromised due to effects such as intensity fluctuation and spectral diffusion caused by interaction with surface states. In this article, a facile, bottom-up technique for the fabrication of sub-10-nm hexagonal boron nitride (hBN) nanoparticles hosting photostable bright emitters via a catalyst-free hydrothermal reaction between boric acid and melamine is demonstrated. A simple stabilization protocol that significantly reduces intensity fluctuation by ≈85% and narrows the emission linewidth by ≈14% by employing a common sol-gel silica coating process is also implemented. This study advances a promising strategy for the scalable, bottom-up synthesis of high-quality quantum emitters in hBN nanoparticles.
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The emergence of interlayer excitons (IEs) from atomic layered transition metal dichalcogenides (TMDCs) heterostructures has drawn tremendous attention due to their unique and exotic optoelectronic properties. Coupling the IEs into optical cavities provides distinctive electromagnetic environments which plays an important role in controlling multiple optical processes such as optical nonlinear generation or photoluminescence enhancement. Here, the integration of IEs in TMDCs into plasmonic nanocavities based on a nanocube on a metallic mirror is reported. Spectroscopic studies reveal an order of magnitude enhancement of the IE at room temperature and a 5-time enhancement in fluorescence at cryogenic temperatures. Cavity modeling reveals that the enhancement of the emission is attributed to both increased excitation efficiency and Purcell effect from the cavity. The results show a novel method to control the excitonic processes in TMDC heterostructures to build high performance photonics and optoelectronics devices.
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Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, but their large spectral variability and unknown local structure challenge their technological utility. Here, we directly correlate hBN quantum emission with local strain using a combination of photoluminescence (PL), cathodoluminescence (CL) and nanobeam electron diffraction. Across 40 emitters, we observe zero phonon lines (ZPLs) in PL and CL ranging from 540 to 720 nm. CL mapping reveals that multiple defects and distinct defect species located within an optically diffraction-limited region can each contribute to the observed PL spectra. Local strain maps indicate that strain is not required to activate the emitters and is not solely responsible for the observed ZPL spectral range. Instead, at least four distinct defect classes are responsible for the observed emission range, and all four classes are stable upon both optical and electron illumination. Our results provide a foundation for future atomic-scale optical characterization of colour centres.