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Optically detected magnetic resonance (ODMR) has become a well-established and powerful technique for measuring the spin state of solid-state quantum emitters, at room temperature. Relying on spin-dependent recombination processes involving the emitters ground, excited and metastable states, ODMR is enabling spin-based quantum sensing of nanoscale electric and magnetic fields, temperature, strain and pressure, as well as imaging of individual electron and nuclear spins. Central to many of these sensing applications is the ability to reliably analyze ODMR data, as the resonance frequencies in these spectra map directly onto target physical quantities acting on the spin sensor. However, this can be onerous, as relatively long integration times -- from milliseconds up to tens of seconds -- are often needed to reach a signal-to-noise level suitable to determine said resonances using traditional fitting methods. Here, we present an algorithm based on data clustering that overcome this limitation and allows determining the resonance frequencies of ODMR spectra with better accuracy (~1.3x factor), higher resolution (~4.7x factor) and/or overall fewer data points (~5x factor) than standard approaches based on statistical inference. The proposed clustering algorithm (CA) is thus a powerful tool for many ODMR-based quantum sensing applications, especially when dealing with noisy and scarce data sets.

Cryogenic temperatures are the prerequisite for many advanced scientific applications and technologies. The accurate determination of temperature in this range and at the submicrometer scale is, however, nontrivial. This is due to the fact that temperature reading in cryogenic conditions can be inaccurate due to optically induced heating. Here, we present an ultralow power, optical thermometry technique that operates at cryogenic temperatures. The technique exploits the temperature dependent linewidth broadening measured by resonant photoluminescence of a two level system, a germanium vacancy color center in a nanodiamond host. The proposed technique achieves a relative sensitivity of 20% 1/K, at 5 K. This is higher than any other all optical nanothermometry method. Additionally, it achieves such sensitivities while employing excitation powers of just a few tens of nanowatts, several orders of magnitude lower than other traditional optical thermometry protocols. To showcase the performance of the method, we demonstrate its ability to accurately read out local differences in temperatures at various target locations of a custom-made microcircuit. Our work is a definite step towards the advancement of nanoscale optical thermometry at cryogenic temperatures.

In recent years, machine and quantum learning have gained considerable momentum sustained by growth in computational power and data availability and have shown exceptional aptness for solving recognition- and classification-type problems, as well as problems that require complex, strategic planning. In this work, we discuss and analyze the role machine and quantum learning are playing in the development of diamond-based quantum technologies. This matters as diamond and its optically-addressable spin defects are becoming prime hardware candidates for solid state-based applications in quantum information, computing and metrology. Through a selected number of demonstrations, we show that machine and quantum learning are leading to both practical and fundamental improvements in measurement speed and accuracy. This is crucial for quantum applications, especially for those where coherence time and signal-to-noise ratio are scarce resources. We summarize some of the most prominent machine and quantum learning approaches that have been conducive to the presented advances and discuss their potential for proposed and future quantum applications., Comment: 31 pages, 3 figures, 1 table

All optical nanothermometry has become a powerful, noninvasive tool for measuring nanoscale temperatures in applications ranging from medicine to nanooptics and solid-state nanodevices. The key features of any candidate nanothermometer are sensitivity and resolution. Here, we demonstrate a real time, diamond based nanothermometry technique with sensitivity and resolution much larger than those of any existing all optical method. The distinct performance of our approach stems from two factors. First, temperature sensors nanodiamonds cohosting two Group IV colour centers engineered to emit spectrally separated Stokes and AntiStokes fluorescence signals under excitation by a single laser source. Second, a parallel detection scheme based on filtering optics and high sensitivity photon counters for fast readout. We demonstrate the performance of our method by monitoring temporal changes in the local temperature of a microcircuit and a MoTe2 field effect transistor. Our work lays the foundation for time resolved temperature monitoring and mapping of micro, nanoscale devices such as microfluidic channels, nanophotonic circuits, and nanoelectronic devices, as well as complex biological environments such as tissues and cells.

Spin defects in solid-state materials are strong candidate systems for quantum information technology and sensing applications. Here we explore in details the recently discovered negatively charged boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) and demonstrate their use as atomic scale sensors for temperature, magnetic fields and externally applied pressure. These applications are possible due to the high-spin triplet ground state and bright spin-dependent photoluminescence (PL) of the $V_B^-$. Specifically, we find that the frequency shift in optically detected magnetic resonance (ODMR) measurements is not only sensitive to static magnetic fields, but also to temperature and pressure changes which we relate to crystal lattice parameters. Our work is important for the future use of spin-rich hBN layers as intrinsic sensors in heterostructures of functionalized 2D materials., Comment: 9 pages, 4 figures, 2 tables

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 letter, we demonstrate a facile, bottom-up technique for the fabrication of sub-10-nm hBN nanoparticles hosting photostable bright emitters via a catalyst-free hydrothermal reaction between boric acid and melamine. We also implement 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. Our study advances a promising strategy for the scalable, bottom-up synthesis of high-quality quantum emitters in hBN nanoparticles.

Optically active defects in solids with accessible spin states are promising candidates for solid state quantum information and sensing applications. To employ these defects as quantum building blocks, coherent manipulation of their spin state is required. Here we realize coherent control of ensembles of boron vacancy (V$_B^-$) centers in hexagonal boron nitride (hBN). Specifically, by applying pulsed spin resonance protocols, we measure spin-lattice relaxation time ($T_1$) of 18 $\mu$s and spin coherence time ($T_2$) of 2 $\mu$s at room temperature. The spin-lattice relaxation time increases by three orders of magnitude at cryogenic temperature. Furthermore, employing a two- and three-pulse electron spin-echo envelope modulation (ESEEM) we separate the quadrupole and hyperfine interactions with the surrounding nuclei. Finally, by applying a method to decouple the spin state from its inhomogeneous nuclear environment - a "hole-burning" - the spectral optically detected magnetic resonance linewidth is significantly reduced to several tens of kHz, thus extending the spin coherence time by a factor of three. Our results are important for employment of van der Waals materials for quantum technologies, specifically in the context of using hBN as a high-resolution quantum sensor for hybrid quantum systems including 2D heterostructures, nanoscale devices and emerging atomically thin magnets.

Extensive photochemical and spectroscopic properties of the $V_B^-$ defect in hexagonal boron nitride are calculated, concluding that the observed photoemission associated with recently observed optically-detected magnetic resonance is most likely of (1)3E" to (1)3A2' origin. Rapid intersystem crossing from the defect's triplet to singlet manifolds explains the observed short excited-state lifetime and very low quantum yield. New experimental results reveal smaller intrinsic spectral bandwidths than previously recognized, interpreted in terms spectral narrowing and zero-phonon-line shifting induced by the Jahn-Teller effect. Different types of computational methods are applied to map out the complex triplet and singlet defect manifolds, including the doubly ionised formulation of the equation-of-motion coupled-cluster theory that is designed to deal with the open-shell nature of defect states, and mixed quantum-mechanics/molecular-mechanics schemes enabling 5763-atom simulations. Two other energetically feasible spectral assignments from amongst the singlet and triplet manifolds are considered, but ruled out based on inappropriate photochemical properties.

Two-dimensional hexagonal boron nitride offers intriguing opportunities for advanced studies of light-matter interaction at the nanoscale, specifically for realizations in quantum nanophotonics. Here, we demonstrate the engineering of optically-addressable spin defects based on the negatively-charged boron vacancy center. We show that these centers can be created in exfoliated hexagonal boron nitride using a variety of focused ion beams (nitrogen, xenon and argon), with nanoscale precision. Using a combination of laser and resonant microwave excitation, we carry out optically detected magnetic resonance spectroscopy measurements, which reveal a zero-field ground state splitting for the defect of ~3.46 GHz. We also perform photoluminescence excitation spectroscopy and temperature dependent photoluminescence measurements to elucidate the photophysical properties of the center. Our results are important for advanced quantum and nanophotonics realizations involving manipulation and readout of spin defects in hexagonal boron nitride.

Nanoscale optical thermometry is a promising non-contact route for measuring local temperature with both high sensitivity and spatial resolution. In this work, we present a deterministic optical thermometry technique based on quantum emitters in nanoscale hexagonal boron-nitride. We show that these nanothermometers exhibit better performance than that of homologous, all-optical nanothermometers both in sensitivity and range of working temperature. We demonstrate their effectiveness as nanothermometers by monitoring the local temperature at specific locations in a variety of custom-built micro-circuits. This work opens new avenues for nanoscale temperature measurements and heat flow studies in miniaturized, integrated devices.

Single photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered significant 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 and by comparing various synthesis methods, we provide direct evidence that the visible SPEs are carbon related. Room temperature optically detected magnetic resonance (ODMR) is demonstrated on ensembles of these defects. We also perform ion implantation experiments and confirm that only carbon implantation creates SPEs in the visible spectral range. Computational analysis of hundreds of potential carbon-based defect transitions suggest that the emission results from the negatively charged VBCN- defect, which experiences long-range out-of-plane deformations and is 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 deterministic engineering of these defects for quantum photonic devices.

Modifying material properties at the nanoscale is crucially important for devices in nanoelectronics, nanophotonics and quantum information. Optically active defects in wide band gap materials, for instance, are vital constituents for the realisation of quantum technologies. Yet, the introduction of atomic defects through direct ion implantation remains a fundamental challenge. Herein, we establish a universal method for material doping by exploiting one of the most fundamental principles of physics - momentum transfer. As a proof of concept, we direct-write arrays of emitters into diamond via momentum transfer from a Xe+ focused ion beam (FIB) to thin films of the group IV dopants pre-deposited onto a diamond surface. We conclusively show that the technique, which we term knock-on doping, can yield ultra-shallow dopant profiles localized to the top 5 nm of the target surface, and use it to achieve sub-50 nm lateral resolution. The knock-on doping method is cost-effective, yet very versatile, powerful and universally suitable for applications such as electronic and magnetic doping of atomically thin materials and engineering of near-surface states of semiconductor devices.

Energy transfer between fluorescent probes lies at the heart of many applications ranging from bio-sensing and -imaging to enhanced photo-detection and light harvesting. In this work, we study F\"orster resonance energy transfer (FRET) between shallow defects in diamond --- nitrogen-vacancy (NV) centers --- and atomically-thin, two-dimensional materials --- tungsten diselenide (WSe$_2$). By means of fluorescence lifetime imaging, we demonstrate the occurrence of FRET in the WSe$_2$/NV system. Further, we show that in the coupled system, NV centers provide an additional excitation pathway for WSe$_2$ photoluminescence. Our results constitute the first step towards the realization of hybrid quantum systems involving single-crystal diamond and two-dimensional materials that may lead to new strategies for studying and controlling spin transfer phenomena and spin valley physics., Comment: v2: accepted for publication in Advanced Quantum Technologies

Integrated quantum photonic circuitry is an emerging topic that requires efficient coupling of quantum light sources to waveguides and optical resonators. So far, great effort has been devoted to engineering on-chip systems from three-dimensional crystals such as diamond or gallium arsenide. In this study, we demonstrate room temperature coupling of quantum emitters embedded within a layered hexagonal boron nitride to an on-chip aluminium nitride waveguide. We achieved 1.2% light coupling efficiency of the device and realise transmission of single photons through the waveguide. Our results serve as a foundation for the integration of layered materials with on-chip components and for the realisation of integrated quantum photonic circuitry.

Diamond photonics is an ever growing field of research driven by the prospects of harnessing diamond and its colour centres as suitable hardware for solid-state quantum applications. The last two decades have seen the field been shaped by the nitrogen-vacancy (NV) centre both with breakthrough fundamental physics demonstrations and practical realizations. Recently however, an entire suite of other diamond defects has emerged. They are M V colour centres, where M indicates one of the elements in the IV column of the periodic table Si, Ge, Sn and Pb, and V indicates lattice vacancies, i.e. missing next-neighbour carbon atoms. These centres exhibit a much stronger emission into the zero phonon line then the NV centre, they display inversion symmetry, and can be engineered using ion implantation all attractive features for scalable quantum photonic architectures based on solid-state, single-photon sources. In this perspective, we highlight the leading techniques for engineering and characterizing these diamond defects, discuss the current state-of-the-art of group IV-based devices and provide an outlook of the future directions the field is taking towards the realisation of solid-state quantum photonics with diamond.

Optically addressable spins in widebandgap semiconductors have become one of the most prominent platforms for exploring fundamental quantum phenomena. While several candidates in 3D crystals including diamond and silicon carbide have been extensively studied, the identification of spindependent processes in atomically thin 2D materials has remained elusive. Although optically accessible spin states in hBN are theoretically predicted, they have not yet been observed experimentally. Here, employing rigorous electron paramagnetic resonance techniques and photoluminescence spectroscopy, we identify fluorescence lines in hexagonal boron nitride associated with a particular defect, the negatively charged boron vacancy and determine the parameters of its spin Hamiltonian. We show that the defect has a triplet ground state with a zero field splitting of 3.5 GHz and establish that the centre exhibits optically detected magnetic resonance at room temperature. We also demonstrate the spin polarization of this centre under optical pumping, which leads to optically induced population inversion of the spin ground state a prerequisite for coherent spin manipulation schemes. Our results constitute a leap forward in establishing two dimensional hBN as a prime platform for scalable quantum technologies, with extended potential for spin based quantum information and sensing applications, as our ODMR studies on hBN NV diamonds hybrid structures show.

Solid-state quantum emitters are garnering a lot of attention due to their role in scalable quantum photonics. A notable majority of these emitters, however, exhibit spectral diffusion due to local, fluctuating electromagnetic fields. In this work, we demonstrate efficient Anti-Stokes (AS) excitation of quantum emitters in hexagonal boron nitride (hBN), and show that the process results in the suppression of a specific mechanism responsible for spectral diffusion of the emitters. We also demonstrate an all-optical gating scheme that exploits Stokes and Anti-Stokes excitation to manipulate spectral diffusion so as to switch and lock the emission energy of the photon source. In this scheme, reversible spectral jumps are deliberately enabled by pumping the emitter with high energy (Stokes) excitation; AS excitation is then used to lock the system into a fixed state characterized by a fixed emission energy. Our results provide important insights into the photophysical properties of quantum emitters in hBN, and introduce a new strategy for controlling the emission wavelength of quantum emitters.

Single-photon emitters in gallium nitride (GaN) are gaining interest as attractive quantum systems due to the well-established techniques for growth and nanofabrication of the host material, as well as its remarkable chemical stability and optoelectronic properties. We investigate the nature of such single-photon emitters in GaN with a systematic analysis of various samples produced under different growth conditions. We explore the effect that intrinsic structural defects (dislocations and stacking faults), doping and crystal orientation in GaN have on the formation of quantum emitters. We investigate the relationship between the position of the emitters (determined via spectroscopy and photoluminescence measurements) and the location of threading dislocations (characterised both via atomic force microscopy and cathodoluminescence). We find that quantum emitters do not correlate with stacking faults or dislocations; instead, they are more likely to originate from point defects or impurities whose density is modulated by the local extended defect density.

Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method employed to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems, and harness it towards the realization of practical nanoscale thermometry and sensing.

Two-dimensional transition-metal dichalcogenides (TMDC) are of great interest for on-chip nanophotonics due to their unique optoelectronic properties. Here, we propose and realize coupling of tungsten diselenide (WSe2) monolayers to circular Bragg grating structures to achieve enhanced emission. The interaction between WSe2 and the resonant mode of the structure results in Purcell-enhanced emission, while the symmetric geometrical structure improves the directionality of the out-coupling stream of emitted photons. Furthermore, this hybrid structure produces a record high contrast of the spin valley readout (> 40%) revealed by the polarization resolved photoluminescence (PL) measurements. Our results are promising for on-chip integration of TMDC monolayers with optical resonators for nanophotonic circuits.

Quantum technologies require robust and photostable single photon emitters (SPEs) that can be reliably engineered. Hexagonal boron nitride (hBN) has recently emerged as a promising candidate host to bright and optically stable SPEs operating at room temperature. However, the emission wavelength of the fluorescent defects in hBN has, to date, been shown to be uncontrolled. The emitters usually display a large spread of zero phonon line (ZPL) energies spanning over a broad spectral range (hundreds of nanometers), which hinders the potential development of hBN-based devices and applications. We demonstrate bottom-up, chemical vapor deposition growth of large-area, few layer hBN that hosts large quantities of SPEs: 100 per 10x10 {\mu}m2. Remarkably, more than 85 percent of the emitters have a ZPL at (580{\pm}10)nm, a distribution which is over an order of magnitude narrower than previously reported. Exploiting the high density and uniformity of the emitters, we demonstrate electrical modulation and tuning of the ZPL emission wavelength by up to 15 nm. Our results constitute a definite advancement towards the practical deployment of hBN single photon emitters in scalable quantum photonic and hybrid optoelectronic devices based on 2D materials.

Layered van der Waals materials are emerging as compelling two-dimensional (2D) platforms for studies of nanophotonics, polaritonics, valleytronics and spintronics, and have the potential to transform applications in sensing, imaging and quantum information processing. Amongst these, hexagonal boron nitride (hBN) is unique in that it hosts ultra-bright, room temperature single photon emitters (SPEs). However, an outstanding challenge is to locate SPEs in hBN with high precision, a task which requires breaking the optical diffraction limit. Here, we report the imaging of SPEs in layered hBN with a spatial resolution of 63 nm using ground state depletion (GSD) nanoscopy. Furthermore, we show that SPEs in hBN possess nonlinear photophysical properties which can be used to realize a new variant of GSD that employs a coincident pair of doughnut-shaped lasers to reduce the laser power that is needed to achieve a given resolution target. Our findings expand the current understanding of the photophysics of quantum emitters in layered hBN and demonstrate the potential for advanced nanophotonic and bio-imaging applications which require localization of individual emitters with super-resolution accuracy.

In this work, we present a detailed photophysical analysis of recently-discovered optically stable, single photon emitters (SPEs) in Gallium Nitride (GaN). Temperature-resolved photoluminescence measurements reveal that the emission lines at 4 K are three orders of magnitude broader than the transform-limited widths expected from excited state lifetime measurements. The broadening is ascribed to ultra-fast spectral diffusion. Continuing the photophysics study on several emitters at room temperature (RT), a maximum average brightness of ~427 kCounts/s is measured. Furthermore, by determining the decay rates of emitters undergoing three-level optical transitions, radiative and non-radiative lifetimes are calculated at RT. Finally, polarization measurements from 14 emitters are used to determine visibility as well as dipole orientation of defect systems within the GaN crystal. Our results underpin some of the fundamental properties of SPE in GaN both at cryogenic and RT, and define the benchmark for future work in GaN-based single-photon technologies.

Solid state single photon emitters (SPEs) are one of the prime components of many quantum nanophotonics devices. In this work, we report on an unusual, photo-induced blinking phenomenon of SPEs in gallium nitride (GaN). This is shown to be due to the modification in the transition kinetics of the emitter, via the introduction of additional laser-activated states. We investigate and characterize the blinking effect on the brightness of the source and the statistics of the emitted photons. Combining second-order correlation and fluorescence trajectory measurements, we determine the photo-dynamics of the trap states and characterize power dependent decay rates and characteristic off-time blinking. Our work sheds new light into understanding solid-state quantum system dynamics and, specifically, power-induced blinking phenomena in SPEs., Comment: Final version appeared in Phys. Rev. B 96, 041203(R) (2017)

Single photon emitters with narrow linewidths are highly sought after for applications in quantum information processing and quantum communications. In this letter, we report on a bright, highly polarized near infrared single photon emitter embedded in diamond nanocrystals with a narrow, sub GHz optical linewidths at 10K. The observed zero phonon line at ~ 780 nm is optically stable under low power resonant excitation and blue shifts as the excitation power increases. Our results highlight the prospect for using new near infrared color centers in nanodiamonds for quantum applications.

We report the observation of room-temperature superradiance from single, highly luminescent diamond nanocrystals with spatial dimensions much smaller than the wavelength of light, and each containing a large number (~10^3) of embedded nitrogen-vacancy (NV) centres. After excitation of the nanodiamonds with an off-resonant, green laser pulse, we observe i) ultrafast radiative lifetimes down to ~ 1 ns, and ii) super-Poissonian photon bunching in the autocorrelation function of the light emitted from the fastest nanodiamonds. We explain our findings with a detailed theoretical model based on collective Dicke states and well-known properties of NV centres. Using a minimal set of fit parameters, the model captures both the wide range of different lifetimes and the nontrivial photon correlations found in the experiments. The results pave the way towards a systematic study of superradiance in a well controlled, solid-state quantum system at room temperature. Ultimately, quantum engineering of superradiance in diamond has the potential for advancing applications in quantum sensing, energy harvesting, and efficient photon detection., Comment: Main text + Supplementary: 12 pages, 7 figures

Colour centres in diamond are promising candidates as a platform for quantum technologies and biomedical imaging based on spins and/or photons. Controlling the emission properties of colour centres in diamond is a key requirement for developing efficient single photon sources with high collection efficiency. A number of groups have produced enhancement in the emission rate over narrow wavelength ranges by coupling single emitters in nanodiamond crystals to resonant electromagnetic structures. Here we characterise in detail the spontaneous emission rates of nitrogen-vacancy centres positioned in various locations on a structured substrate. We show an average factor of 1.5 enhancement of the total emission rate when nanodiamonds are on an opal photonic crystal surface, and observe changes in the lifetime distribution. We present a model to explain these observations and associate the lifetime properties with dipole orientation and polarization effects., Comment: 16 pages, 10 figures

Fluorescent defects in non-cytotoxic diamond nanoparticles are candidates for qubits in quantum computing, optical labels in biomedical imaging and sensors in magnetometry. For each application these defects need to be optically and thermodynamically stable, and included in individual particles at suitable concentrations (singly or in large numbers). In this letter, we combine simulations, theory and experiment to provide the first comprehensive and generic prediction of the size, temperature and nitrogen-concentration dependent stability of optically active NV defects in nanodiamonds., Comment: Published in Nano Letters August 2009 24 pages, 6 figures