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Group IV color centers in diamond are among the most promising optically active spin systems with strong optical transitions and long spin coherences. The ground-state splitting of the center is particularly important to suppress the interaction with coherence-limiting phonons, which improves the coherence properties and sets the upper limit for the operating temperature. Negatively charged silicon-vacancy centers have an ordinary ground-state splitting of only 48GHz, resulting in required temperatures below one Kelvin, which can only be achieved by dilution refrigerators. Here, we increase the ground-state splitting by up to an order of magnitude by induced strain in a single-crystal diamond membrane. Furthermore, we demonstrate cavity-assisted spectroscopy enabled by coupling the emitter ensemble with a selectable strain to the mode of a Fabry-Perot microcavity. Calculation of the absorption cross-section yields $\sigma_{ens} = $4.9*10^-11 cm^2. Together with the Purcell-enhanced twofold reduction in emitter lifetime below 1ns, this makes the system a promising spin-photon interface at moderate temperatures of 4K., Comment: 12 pages, 9 figures

Among the wealth of single fluorescent defects recently detected in silicon, the G center catches interest for its telecom single-photon emission that could be coupled to a metastable electron spin triplet. The G center is a unique defect where the standard Born-Oppenheimer approximation breaks down as one of its atoms can move between 6 lattice sites under optical excitation. The impact of this atomic reconfiguration on the photoluminescence properties of G centers is still largely unknown, especially in silicon-on-insulator (SOI) samples. Here, we investigate the displacement of the center-of-mass of the G center in silicon. We show that single G defects in SOI exhibit a multipolar emission and zero-phonon line fine structures with splittings up to $\sim1$ meV, both indicating a motion of the defect central atom over time. Combining polarization and spectral analysis at the single-photon level, we evidence that the reconfiguration dynamics are drastically different from the one of the unperturbed G center in bulk silicon. The SOI structure freezes the delocalization of the G defect center-of-mass and as a result, enables to isolate linearly polarized optical lines. Under above-bandgap optical excitation, the central atom of G centers in SOI behaves as if it were in a 6-slot roulette wheel, randomly alternating between localized crystal sites at each optical cycle. Comparative measurements in a bulk silicon sample and ab initio calculations highlight that strain is likely the dominant perturbation impacting the G center geometry. These results shed light on the importance of the atomic reconfiguration dynamics to understand and control the photoluminescence properties of the G center in silicon. More generally, these findings emphasize the impact of strain fluctuations inherent to SOI wafers for future quantum integrated photonics applications based on color centers in silicon.

Group-IV color centers in diamond are promising candidates for quantum networks due to their dominant zero-phonon line and symmetry-protected optical transitions that connect to coherent spin levels. The negatively charged tin-vacancy (SnV) center possesses long electron spin lifetimes due to its large spin-orbit splitting. However, the magnetic dipole transitions required for microwave spin control are suppressed, and strain is necessary to enable these transitions. Recent work has shown spin control of strained emitters using microwave lines that suffer from Ohmic losses, restricting coherence through heating. We utilize a superconducting coplanar waveguide to measure SnV centers subjected to strain, observing substantial improvement. A detailed analysis of the SnV center electron spin Hamiltonian based on the angle-dependent splitting of the ground and excited states is performed. We demonstrate coherent spin manipulation and obtain a Hahn echo coherence time of up to $T_2 = 430\,\mu$s. With dynamical decoupling, we can prolong coherence to $T_2 = 10\,$ms, about six-fold improved compared to earlier works. We also observe a nearby coupling $^{13}\mathrm{C}$ spin which may serve as a quantum memory. This substantiates the potential of SnV centers in diamond and demonstrates the benefit of superconducting microwave structures., Comment: Main: 9 pages, 5 figures, 1 tables; Supplement: 15 pages, 10 figures, 1 table

Among the wide variety of single fluorescent defects investigated in silicon, numerous studies have focused on color centers with a zero-phonon line around $1.28 \mu$m and identified to a common carbon-complex in silicon, namely the G center. However, inconsistent estimates regarding their quantum efficiency cast doubt on the correct identification of these individual emitters. Through a comparative analysis of their single-photon emission properties, we demonstrate that these single color centers are split in two distinct families of point defects. A first family consists of the genuine single G centers with a well-identified microscopic structure and whose photoluminescence has been investigated on ensemble measurements since the 60's. The remaining defects belong to a new color center, which we will refer to as G$^{\star}$ center, whose atomic configuration has yet to be determined. These results provide a safeguard against future defect misidentifications, which is crucial for further development of quantum technologies relying on G or G$^{\star}$ center quantum properties.

The creation of fluorescent defects in silicon is a key stepping stone towards assuring the integration perspectives of quantum photonic devices into existing technologies. Here we demonstrate the creation, by femtosecond laser annealing, of W and G-centers in commercial silicon on insulator (SOI) previously implanted with 12C+ ions. Their quality is comparable to that found for the same emitters obtained with conventional implant processes; as quantified by the photoluminescence radiative lifetime, the broadening of their zero-phonon line (ZPL) and the evolution of these quantities with temperature. In addition to this, we show that both defects can be created without carbon implantation and that we can erase the G-centers by annealing while enhancing the W-centers' emission. These demonstrations are relevant to the deterministic and operando generation of quantum emitters in silicon., Comment: 8 pages, 4 figures

An important tool in the investigation of the early stages of neurodegenerative disease is the study of dissected living tissue from the brain of an animal model. Such investigations allow the physical structure of individual neurons and neural circuits to be probed alongside neuronal electrical activity, disruption of which can shed light on the mechanisms of emergence of disease. Existing techniques for recording activity rely on potentially damaging direct interaction with the sample, either mechanically as point electrical probes or via intense focused laser light combined with highly specific genetic modification and/or potentially toxic fluorescent dyes. In this work, we instead perform passive, microscopic-scale recording of electrical activity using a biocompatible quantum sensor based on colour centres in diamond. We record biomagnetic field induced by ionic currents in mouse corpus callosum axons without direct sample interaction, accurately recovering signals corresponding to action potential propagation while demonstrating in situ pharmacology during biomagnetic recording through tetrodotoxin inhibition of voltage gated sodium channels. Our results open a promising new avenue for the microscopic recording of neuronal signals, offering the prospect of high resolution imaging of electrical circuits in the living mammalian brain.

We report the fabrication of G centers in silicon with an areal density compatible with single photon emission at optical telecommunication wavelengths. Our sample is made from a silicon-on-insulator wafer which is locally implanted with carbon ions and protons at various fluences. Decreasing the implantation fluences enables to gradually switch from large ensembles to isolated single defects, reaching areal densities of G centers down to $\sim$0.2 $\mu$m$^{-2}$. Single defect creation is demonstrated by photon antibunching in intensity-correlation experiments, thus establishing our approach as a reproducible procedure for generating single artificial atoms in silicon for quantum technologies.

Defect engineering is foundational to classical electronic device development and for emerging quantum devices. Here, we report on defect engineering of silicon single crystals with ion pulses from a laser accelerator with ion flux levels up to 10^22 ions/cm^2/s. Low energy ions from plasma expansion of the laser-foil target are implanted near the surface and then diffuse into silicon samples that were locally pre-heated by high energy ions. We observe low energy ion fluences of ~10^16 cm^-2, about four orders of magnitude higher than the fluence of high energy (MeV) ions. In the areas of highest energy deposition, silicon crystals exfoliate from single ion pulses. Color centers, predominantly W and G-centers, form directly in response to ion pulses without a subsequent annealing step. We find that the linewidth of G-centers increase in areas with high ion flux much more than the linewidth of W-centers, consistent with density functional theory calculations of their electronic structure. Laser ion acceleration generates aligned pulses of high and low energy ions that expand the parameter range for defect engineering and doping of semiconductors with tunable balances of ion flux, damage rates and local heating.

The detection of physiological activity at the microscopic level is key for understanding the function of biosystems and relating this to physical structure. Current sensing methods often rely on invasive probes to stimulate and detect activity, bearing the risk of inducing damage in the target system. In recent years, a new type of biosensor based on color centers in diamond offers the possibility to passively, noninvasively sense and image living biological systems. Here, we use such a sensor for the \textit{in-vitro} recording of the local magnetic field generated by tightly focused, high intensity pulsed laser optogenetic neuromuscular stimulation of the extensor digitorum longus muscles. Recordings captured a compound action potential response and a slow signal component which we seek to explain using a detailed model of the biological system. We show that our sensor is capable of recording localized neuromuscular activity from the laser stimulation site without photovoltaic or fluorescence artifacts associated with alternative techniques. Our work represents an important step towards selective induction of localized neurobiological activity while performing passive sensing and imaging with diamond sensors, motivating further research into mapping of neural activity and intra-cellular processes.

In this work, we demonstrate that cutting diamond crystals with a laser (532~nm wavelength, 0.5~mJ energy, 200~ns pulse duration at 15~kHz) produces a $\lesssim 20~$nm thick surface layer with magnetic order at room temperature. We have measured the magnetic moment of five natural and six CVD diamond crystals of different size, nitrogen content and surface orientations with a SQUID magnetometer. A robust ferromagnetic response at 300~K is observed only for crystals that were cut with the laser along the (100) surface orientation. The magnetic signals are much weaker for the (110) and negligible for the (111) orientations. We attribute the magnetic order to the disordered graphite layer produced by the laser at the diamond surface. The ferromagnetic signal vanished after chemical etching or after moderate temperature annealing. The obtained results indicate that laser treatment of diamond may pave the way to create ferromagnetic spots at its surface., Comment: 8 pages with 8 figures

Several diamond bulk crystals with a concentration of electrically neutral single substitutional nitrogen atoms of $\lesssim 80~$ppm, the so-called C- or P1-centres, were irradiated with electrons at 10 MeV energy and low fluence. The results show a complete suppression of the irreversible behavior in field and temperature of the magnetization below $\sim 30$~K, after a decrease of $\lesssim 40~$ppm in the concentration of C-centres produced by the electron irradiation. This result indicates that magnetic C-centres are at the origin of the large hysteretic behavior found recently in nitrogen-doped diamond crystals. This is remarkable because of the relatively low density of C-centres, stressing the extraordinary role of the C-centres in triggering those phenomena in diamond at relatively high temperatures. After annealing the samples at high temperatures in vacuum, the hysteretic behavior is partially recovered., Comment: 15 pages, 10 figures

Controlling the quantum properties of individual fluorescent defects in silicon is a key challenge towards advanced quantum photonic devices prone to scalability. Research efforts have so far focused on extrinsic defects based on impurities incorporated inside the silicon lattice. Here we demonstrate the detection of single intrinsic defects in silicon, which are linked to a tri-interstitial complex called W-center, with a zero-phonon line at 1.218${\mu}$m. Investigating their single-photon emission properties reveals new information about this common radiation damage center, such as its dipolar orientation and its photophysics. We also identify its microscopic structure and show that although this defect does not feature electronic states in the bandgap, Coulomb interactions lead to excitonic radiative recombination below the silicon bandgap. These results could set the stage for numerous quantum perspectives based on intrinsic luminescent defects in silicon, such as quantum integrated photonics, quantum communications and quantum sensing.

The ability to measure the passage of electrical current with high spatial and temporal resolution is vital for applications ranging from inspection of microscopic electronic circuits to biosensing. Being able to image such signals passively and remotely at the same time is of high importance, to measure without invasive disruption of the system under study or the signal itself. A new approach to achieve this utilises point defects in solid state materials, in particular nitrogen vacancy (NV) centres in diamond. Acting as a high density array of independent sensors, addressable opto-electronically and highly sensitive to factors including temperature and magnetic field, these are ideally suited to microscopic widefield imaging. In this work we demonstrate such imaging of signals from a microscopic lithographically patterned circuit at the micrometer scale. Using a new type of lock-in amplifier camera, we demonstrate sub-millisecond (up to 3500 frames-per-second) spatially resolved recovery of AC and pulsed electrical current signals, without aliasing or undersampling. Finally, we demonstrate as a proof of principle the recovery of synthetic signals replicating the exact form of signals in a biological neural network: the hippocampus of a mouse.

We report a systematic photoluminescence (PL) investigation of the spectral emission properties of individual optical defects fabricated in diamond upon ion implantation and annealing. Three spectral lines at 620 nm, 631 nm, and 647 nm are identified and attributed to the SnV center due to their occurrence in the PL spectra of the very same single-photon emitting defects. We show that the relative occurrence of the three spectral features can be modified by oxidizing the sample surface following thermal annealing. We finally report the relevant emission properties of each class of individual emitters, including the excited state emission lifetime and the emission intensity saturation parameters., Comment: 12 pages, 6 figures, 1 table

We report on the systematic characterization of the optical properties of diamond color centers based on Pb impurities. An ensemble photoluminescence analysis of their spectral emission was performed at different excitation wavelengths in the 405-520 nm range and at different temperatures in the 4-300 K range. The series of observed spectral features consist of different emission lines associated with Pb-related defects. Finally, a room-temperature investigation of single-photon emitters under 490.5 nm laser excitation is reported, revealing different spectral signatures with respect to those already reported under 514 nm excitation. This work represents a substantial progress with respect to previous studies on Pb-related color centers, both in the attribution of an articulated series of spectral features and in the understanding of the formation process of this type of defect, thus clarifying the potential of this system for high-impact applications in quantum technologies.

An efficient atom-photon-interface is a key requirement for the integration of solid-state emitters such as color centers in diamond into quantum technology applications. Just like other solid state emitters, however, their emission into free space is severely limited due to the high refractive index of the bulk host crystal. In this work, we present a planar optical antenna based on two silver mirrors coated on a thin single crystal diamond membrane, forming a planar Fabry-P\'erot cavity that improves the photon extraction from single tin vacancy (SnV) centers as well as their coupling to an excitation laser. Upon numerical optimization of the structure, we find theoretical enhancements in the collectible photon rate by a factor of 60 as compared to the bulk case. As a proof-of-principle demonstration, we fabricate single crystal diamond membranes with sub-$\mu$m thickness and create SnV centers by ion implantation. Employing off-resonant excitation, we show a 6-fold enhancement of the collectible photon rate, yielding up to half a million photons per second from a single SnV center. At the same time, we observe a significant reduction of the required excitation power in accordance with theory, demonstrating the functionality of the cavity as an optical antenna. Due to its planar design, the antenna simultaneously provides similar enhancements for a large number of emitters inside the membrane. Furthermore, the monolithic structure provides high mechanical stability and straightforwardly enables operation under cryogenic conditions as required in most spin-photon interface implementations., Comment: The following article contains 31 pages and 6 figures and has been submitted to APL Photonics

Nitrogen vacancy (NV) centers in diamond have attracted considerable recent interest for use in quantum sensing, promising increased sensitivity for applications ranging from geophysics to biomedicine. Conventional sensing schemes involve monitoring the change in red fluorescence from the NV center under green laser and microwave illumination. Due to the strong fluorescence background from emission in the NV triplet state and low relative contrast of any change in output, sensitivity is severely restricted by a high optical shot noise level. Here, we propose a means to avoid this issue, by using the change in green pump absorption through the diamond as part of a semiconductor external cavity laser run close to lasing threshold. We show theoretical sensitivity to magnetic field on the pT/sqrt(Hz) level is possible using a diamond with an optimal density of NV centers. We discuss the physical requirements and limitations of the method, particularly the role of amplified spontaneous emission near threshold and explore realistic implementations using current technology.

The ability to perform noninvasive, non-contact measurements of electric signals produced by action potentials is essential in biomedicine. A key method to do this is to remotely sense signals by the magnetic field they induce. Existing methods for magnetic field sensing of mammalian tissue, used in techniques such as magnetoencephalography of the brain, require cryogenically cooled superconducting detectors. These have many disadvantages in terms of high cost, flexibility and limited portability as well as poor spatial and temporal resolution. In this work we demonstrate an alternative technique for detecting magnetic fields generated by the current from action potentials in living tissue using nitrogen vacancy centres in diamond. With 50pT/$\sqrt{Hz}$ sensitivity, we show the first measurements of sensing from mammalian tissue with a diamond sensor using mouse muscle optogenetically activated with blue light. We show these measurements can be performed in an ordinary, unshielded lab environment and that the signal can be easily recovered by digital signal processing techniques.

High-fidelity projective readout of a qubit's state in a single experimental repetition is a prerequisite for various quantum protocols of sensing and computing. Achieving single-shot readout is challenging for solid-state qubits. For Nitrogen-Vacancy (NV) centers in diamond, it has been realized using nuclear memories or resonant excitation at cryogenic temperature. All of these existing approaches have stringent experimental demands. In particular, they require a high efficiency of photon collection, such as immersion optics or all-diamond micro-optics. For some of the most relevant applications, such as shallow implanted NV centers in a cryogenic environment, these tools are unavailable. Here we demonstrate an all-optical spin readout scheme that achieves single-shot fidelity even if photon collection is poor (delivering less than 10$^3$ clicks/second). The scheme is based on spin-dependent resonant excitation at cryogenic temperature combined with spin-to-charge conversion, mapping the fragile electron spin states to the stable charge states. We prove this technique to work on shallow implanted NV centers as they are required for sensing and scalable NV-based quantum registers., Comment: 21 pages including supplementary information; overall improvements

Sensing of signals from biological processes, such as action potential propagation in nerves, are essential for clinical diagnosis and basic understanding of physiology. Sensing can be performed electrically by placing sensor probes near or inside a living specimen or dissected tissue using well established electrophysiology techniques. However, these electrical probe techniques have poor spatial resolution and cannot easily access tissue deep within a living subject, in particular within the brain. An alternative approach is to detect the magnetic field induced by the passage of the electrical signal, giving the equivalent readout without direct electrical contact. Such measurements are performed today using bulky and expensive superconducting sensors with poor spatial resolution. An alternative is to use nitrogen vacancy (NV) centres in diamond that promise biocompatibilty and high sensitivity without cryogenic cooling. In this work we present advances in biomagnetometry using NV centres, demonstrating magnetic field sensitivity of approximately 100 pT/$\sqrt{Hz}$ in the DC/low frequency range using a setup designed for biological measurements. Biocompatibility of the setup with a living sample (mouse brain slice) is studied and optimized, and we show work toward sensitivity improvements using a pulsed magnetometry scheme. In addition to the bulk magnetometry study, systematic artifacts in NV-ensemble widefield fluorescence imaging are investigated.

The recently discovered negatively charged tin-vacancy centre in diamond is a promising candidate for applications in quantum information processing (QIP). We here present a detailed spectroscopic study encompassing single photon emission and polarisation properties, the temperature dependence of emission spectra as well as a detailed analysis of the phonon sideband and Debye-Waller factor. Using photoluminescence excitation spectroscopy (PLE) we probe an energetically higher lying excited state and prove fully lifetime limited linewidths of single emitters at cryogenic temperatures. For these emitters we also investigate the stability of the charge state under resonant excitation. These results provide a detailed insight into the spectroscopic properties of the $\text{SnV}^-$ centre and lay the foundation for further studies regarding its suitability in QIP.

Nitrogen-vacancy (NV) centers feature outstanding properties like a spin coherence time of up to one second as well as a level structure offering the possibility to initialize, coherently manipulate and optically read-out the spin degree of freedom of the ground state. However, only about three percent of their photon emission are channeled into the zero phonon line (ZPL), limiting both the rate of indistinguishable single photons and the signal-to-noise ratio (SNR) of coherent spin-photon interfaces. We here report on the enhancement of the SNR of the optical spin read-out achieved by tuning the mode of a two-dimensional photonic crystal (PhC)cavity into resonance with the NV-ZPL. PhC cavities are fabricated by focused ion beam (FIB) milling in thin reactive ion (RIE) etched ultrapure single crystal diamond membranes featuring modes with Q-factors of up to 8250 at mode volumes below one cubic wavelength. NV centers are produced in the cavities in a controlled fashion by a high resolution atomic force microscope (AFM) implantation technique. On cavity resonance we observe a lifetime shortening from 9.0ns to 8.0ns as well as an enhancement of the ZPL emission by almost one order of magnitude. Although on resonance the collection efficiency of ZPL photons and the spin-dependent fluorescence contrast are reduced, the SNR of the optical spin read-out is almost tripled for the cavity-coupled NV centers.

Understanding the mechanisms behind high-$T_{c}$ Type-II superconductors (SC) is still an open task in condensed matter physics. One way to gain further insight into the microscopic mechanisms leading to superconductivity is to study the magnetic properties of the SC in detail, for example by studying the properties of vortices and their dynamics. In this work we describe a new method of wide-field imaging magnetometry using nitrogen-vacancy (NV) centers in diamond to image vortices in an yttrium barium copper oxide (YBCO) thin film. We demonstrate quantitative determination of the magnetic field strength of the vortex stray field, the observation of vortex patterns for different cooling fields and direct observation of vortex pinning in our disordered YBCO film. This method opens prospects for imaging of the magnetic-stray fields of vortices at frequencies from DC to several megahertz within a wide range of temperatures which allows for the study of both high-$T_{C}$ and low-$T_{C}$ SCs. The wide temperature range allowed by NV center magnetometry also makes our approach applicable for the study of phenomena like island superconductivity at elevated temperatures (e.g. in metal nano-clusters)., Comment: Main text (4 pages, 3 figures)

We demonstrate a technique for precision sensing of temperature or the magnetic field by simultaneously driving two hyperfine transitions involving distinct electronic states of the nitrogen-vacancy center in diamond. Frequency modulation of both driving fields is used with either the same or opposite phase, resulting in the immunity to fluctuations in either the magnetic field or the temperature, respectively. In this way, a sensitivity of 1.4 nT Hz$^{-1/2}$ or 430 $\mu$K Hz$^{-1/2}$ is demonstrated. The presented technique only requires a single frequency demodulator and enables the use of phase-sensitive camera imaging sensors. A simple extension of the method utilizing two demodulators allows for simultaneous, independent, and high-bandwidth monitoring of both the magnetic field and temperature., Comment: 5 pages, 4 figures

In this work we investigated the time behavior of the polarization of bulk 13C nuclei in diamond above the thermal equilibrium. This nonthermal nuclear hyperpolarization is achieved by cross relaxation between two nitrogen related paramagnetic defect species in diamond in combination with optical pumping. The decay of the hyperpolarization at four different magnetic fields is measured. Furthermore, we use the comparison with conventional nuclear resonance measurements to identify the involved distances of the nuclear spin with respect to the defects and therefore the coupling strengths. Also, a careful look at the linewidth of the signal give valuable information to piece together the puzzle of the hyperpolarization mechanism.

Detecting and controlling nuclear spin nano-ensembles is crucial for the further development of nuclear magnetic resonance (NMR) spectroscopy and for the emerging solid state quantum technology. Here we present the fabrication of a $\approx$ 1 nanometre thick diamond layer consisting of $^{13}$C nuclear spins doped with Nitrogen-Vacancy centres (NV) embedded in a spin-free $^{12}$C crystal matrix. A single NV in the vicinity of the layer is used for polarization of the $^{13}$C spins and the readout of their magnetization. We demonstrate a method for coherent control of few tens of nuclear spins by using radio frequency pulses and show the basic coherent control experiments - Rabi oscillations, Ramsey spectroscopy and Hahn echo, though any NMR pulse sequence can be implemented. The results shown present a first steps towards the realization of a nuclear spin based quantum simulator.

In this work we have used focused electron beam induced deposition of cobalt to functionalize atomic force microscopy Akiyama tips for application in magnetic force microscopy. The grown tips have a content of 90% Co after exposure to ambient air. The magnetic tips were characterized using energy dispersive X-ray spectroscopy and scanning electron microscopy. In order to investigate the magnetic properties, current loops were prepared by electron beam lithography. Measurements at room temperature as well as 4.2K were carried out and the coercive field of 68 Oe of the Co tip was estimated by applying several external fields in the opposite direction of the tip magnetization. Magnetic Akiyama tips open new possibilities for low to room-temperature magnetic force microscopy measurements.

Sensitive, real-time optical magnetometry with nitrogen-vacancy centers in diamond relies on accurate imaging of small ($\ll 10^{-2}$) fractional fluorescence changes across the diamond sample. We discuss the limitations on magnetic-field sensitivity resulting from the limited number of photoelectrons that a camera can record in a given time. Several types of camera sensors are analyzed and the smallest measurable magnetic-field change is estimated for each type. We show that most common sensors are of a limited use in such applications, while certain highly specific cameras allow to achieve nanotesla-level sensitivity in $1$~s of a combined exposure. Finally, we demonstrate the results obtained with a lock-in camera that pave the way for real-time, wide-field magnetometry at the nanotesla level and with micrometer resolution., Comment: 7 pages, 4 figures

Precise timekeeping is critical to metrology, forming the basis by which standards of time, length and fundamental constants are determined. Stable clocks are particularly valuable in spectroscopy as they define the ultimate frequency precision that can be reached. In quantum metrology, where the phase of a qubit is used to detect external fields, the clock stability is defined by the qubit coherence time, which determines the spectral linewidth and frequency precision. Here we demonstrate a quantum sensing protocol where the spectral precision goes beyond the sensor coherence time and is limited by the stability of a classical clock. Using this technique, we observe a precision in frequency estimation scaling in time $T$, as $T^{-3/2}$ for classical oscillating fields. The narrow linewidth magnetometer based on single spins in diamond is used to sense nanoscale magnetic fields with an intrinsic frequency resolution of 607 $\mu$Hz, 8 orders of magnitude narrower than the qubit coherence time., Comment: Related work: Boss et. al., 10.1126/science.aam7009; Bucher et. al., arXiv:1705.08887. Supplementary Information available at: www.sciencemag.org/content/356/6340/832/suppl/DC1

Water is the most important solvent in nature. It is a crucial issue to study interactions among water molecules. Nuclear magnetic resonance (NMR) spectroscopy is one of the most powerful tools to detect magnetic interactions for the structure analysis of a molecule with broad applications. But conventional NMR spectroscopy requires macroscopic sample quantities with hampers in investigating nanoscale structures. Through quantum control of a single spin quantum sensor, magnetic resonance spectroscopy of nanoscale organic molecules and single molecules has been achieved. However, the measurement of the dipolar interaction of nuclear spins within a molecule at nanoscale and the analysis of its structure remain a big challenge. Here we succeed in detecting the NMR spectrum from an ice crystal with (6-nanometer)$^3$ detection volume. More importantly, the magnetic dipolar coupling between two proton nuclear spins of a water molecule was recorded. The resolved intra-molecule magnetic dipolar interactions are about 15 kHz and 33 kHz with spectral resolution at a few kHz. Analysis of the interaction-resolved NMR spectroscopy provides a spatial view of nanoscale ice crystal, from which the orientation of a water-molecule bond is derived and further the length of the bond can be got. This work enables NMR spectroscopy applications in single molecule structure analysis, provides a further tool for nanocrystalline and confined water research.

Hyperpolarisation at room temperature is one of the most important research fields in order to improve liquid, gas or nanoparticle tracer for Magnetic Resonance Imaging (MRI) in medical applications. In this paper we utilize nuclear magnetic resonance (NMR) to investigate the hyperpolarisation effect of negatively charged nitrogen vacancy (NV) centres on carbon-13 nuclei and their spin diffusion in a diamond single crystal close to the excited state level anti crossing (ESLAC) around 50 mT. Whereas the electron spins of the NV centre can be easily polarized in its m = 0 ground state at room temperature just by irradiation with green light , the swop of the NV electron spin polarization to a carbon-13 nuclei is a complex task. We found that the coupling between the polarized NV electron spin, the electron spin of a substitutional nitrogen impurity (P1) as well as its nitrogen-14 nuclei and the carbon-13 nuclear spin has to be considered. Here we show that through an optimization of this procedure, in about two minutes a signal to noise ratio which corresponds to a 23 hour standard measurement without hyperpolarisation and an accumulation of 460 single scans can be obtained. Furthermore we were able to identify several polarisation peaks of different sign at different magnetic fields in a region of some tens of gauss. Most of the peaks can be attributed to a coupling of the NV centres to nearby P1 centres. We present a new theoretical model in a framework of cross polarisation of a four spin dynamic model in good agreement with our experimental data. The results demonstrate the opportunities and power as well as limitations of hyperpolarisation in diamond via NV centres. We expect that the current work may have a significant impact on future applications.

In recent years, solid-state spin systems have emerged as promising candidates for quantum information processing (QIP). Prominent examples are the Nitrogen-Vacancy (NV) center in diamond, phosphorous dopants in silicon (Si:P), rare-earth ions in solids and V$_{\text{Si}}$-centers in Silicon-carbide (SiC). The Si:P system has demonstrated, that by eliminating the electron spin of the dopant, its nuclear spins can yield exceedingly long spin coherence times. For NV centers, however, a proper charge state for storage of nuclear spin qubit coherence has not been identified yet. Here, we identify and characterize the positively charged NV center as an electron-spin-less and optically inactive state by utilizing the nuclear spin qubit as a probe. We control the electronic charge and spin utilizing nanometer scale gate electrodes. We achieve a lengthening of the nuclear spin coherence times by a factor of 20. Surprisingly, the new charge state allows switching the optical response of single nodes facilitating full individual addressability., Comment: 8 pages, 4 figures, 1 table

Measuring with high precision the electrical resistance of highly ordered natural graphite samples from a Brazil mine, we have identified a transition at $\sim$350~K with $\sim$40~K transition width. The step-like change in temperature of the resistance, its magnetic irreversibility and time dependence after a field change, consistent with trapped flux and flux creep, and the partial magnetic flux expulsion obtained by magnetization measurements, suggest the existence of granular superconductivity below 350~K. The zero-field virgin state can only be reached again after zero field cooling the sample from above the transition. Paradoxically, the extraordinarily high transition temperature we found for this and several other graphite samples is the reason why this transition remained undetected so far. The existence of well ordered rhombohedral graphite phase in all measured samples has been proved by x-rays diffraction measurements, suggesting its interfaces with the Bernal phase as a possible origin for the high-temperature superconductivity, as theoretical studies predicted. The localization of granular superconductivity at these two dimensional interfaces prevents the observation of a zero resistance state or of a full Meissner state., Comment: 14 pages with 21 figures

We present the controlled creation of single nitrogen-vacancy (NV) centers via ion implantation at the center of a photonic crystal cavity which is fabricated in an ultrapure, single crystal diamond membrane. High-resolution placement of NV centers is achieved using collimation of a 5keV-nitrogen ion beam through a pierced tip of an atomic force microscope (AFM). We demonstrate coupling of the implanted NV centers' broad band fluorescence to a cavity mode and observe Purcell enhancement of the spontaneous emission. The results are in good agreement with a master equation model for the cavity coupling., Comment: 4 pages, 3 figures

Single charge detection with nanoscale spatial resolution in ambient conditions is a current frontier in metrology that has diverse interdisciplinary applications. Here, such single charge detection is demonstrated using two nitrogen-vacancy (NV) centers in diamond. One NV center is employed as a sensitive electrometer to detect the change in electric field created by the displacement of a single electron resulting from the optical switching of the other NV center between its neutral (NV$^0$) and negative (NV$^-$) charge states. As a consequence, our measurements also provide direct insight into the charge dynamics inside the material.

Precise control of quantum systems is of fundamental importance for quantum device engineering, such as is needed in the fields of quantum information processing, high-resolution spectroscopy and quantum metrology. When scaling up the quantum registers in such devices, several challenges arise: individual addressing of qubits in a dense spectrum while suppressing crosstalk, creation of entanglement between distant nodes, and decoupling from unwanted interactions. The experimental implementation of optimal control is a prerequisite to meeting these challenges. Using engineered microwave pulses, we experimentally demonstrate optimal control of a prototype solid state spin qubit system comprising thirty six energy levels. The spin qubits are associated with proximal nitrogen-vacancy (NV) centers in diamond. We demonstrate precise single-electron spin qubit operations with an unprecedented fidelity F \approx 0.99 in combination with high-efficiency storage of electron spin states in a nuclear spin quantum memory. Matching single-electron spin operations with spin-echo techniques, we further realize high-quality entangled states (F > 0.82) between two electron spins on demand. After exploiting optimal control, the fidelity is mostly limited by the coherence time and imperfect initialization. Errors from crosstalk in a crowded spectrum of 8 lines as well as detrimental effects from active dipolar couplings have been simultaneously eliminated to unprecedented extent. Finally, by entanglement swapping to nuclear spins, nuclear spin entanglement over a length scale of 25 nm is demonstrated. This experiment underlines the importance of optimal control for scalable room temperature spin-based quantum information devices., Comment: 10+6 pages, 6 figures

The creation of nitrogen-vacancy centres in diamond is nowadays well controlled using nitrogen implantation and annealing. Although the high-resolution placement of NV centres has been demonstrated using either collimation through pierced AFM tips or masks with apertures made by electron beam lithography, a targeted implantation into pre-defined structures in diamond may not be achieved using these techniques. We show that a beam of nitrogen ions can be focused to approximately 100 nm using focused ion beam (FIB) technology. The nitrogen ion beam is produced using an electron cyclotron resonance (ECR) plasma source. Combined with a scanning electron microscope, the nitrogen-FIB offers new possibilities for the targeted creation of single defects in diamond. This maskless technology is suitable for example for the creation of optical centres in the cavities of photonic crystals or in diamond tips for scanning magnetometry. Finally, we further show that by changing the gas source from nitrogen to xenon, standard FIB milling capabilities are also available within the same tool.

Experiments show that shallow nitrogen implantations (<10keV) result in a negatively charged nitrogen-vacancy center (NV-) yield of 0.01-0.1%. The most succesful technique for introducing NV- centers in the carbon matrix is ion implantation followed by annealing at 1100K. We investigated the influence of channeling effects during shallow implantation and statistical diffusion using molecular dynamics (MD) and Monte Carlo (MC) approaches. Energy barriers for the diffusion process were calculated using the density functional theory (DFT). Our simulations show a significant difference in the NV yield compared to the experiment. Statistically, 25% of the implanted nitrogens form a NV center after annealing., Comment: 5 pages, 6 figures

Entanglement is the central yet fleeting phenomena of quantum physics. Once being considered a peculiar counter-intuitive property of quantum theory it has developed into the most central element of quantum technology providing speed up to quantum computers, a path towards long distance quantum cryptography and increased sensitivity in quantum metrology. Consequently, there have been a number of experimental demonstration of entanglement between photons, atoms, ions as well as solid state systems like spins or quantum dots, superconducting circuits and macroscopic diamond. Here we experimentally demonstrate entanglement between two engineered single solid state spin quantum bits (qubits) at ambient conditions. Photon emission of defect pairs reveals ground state spin correlation. Entanglement (fidelity = 0.67 \pm 0.04) is proven by quantum state tomography. Moreover, the lifetime of electron spin entanglement is extended to ms by entanglement swapping to nuclear spins, demonstrating nuclear spin entanglement over a length scale of 25 nm. The experiments mark an important step towards a scalable room temperature quantum device being of potential use in quantum information processing as well as metrology.

We present investigations on single Ni/Si related color centers produced via ion implantation into single crystalline type IIa CVD diamond. Testing different ion dose combinations we show that there is an upper limit for both the Ni and the Si dose 10^12/cm^2 and 10^10/cm^2 resp.) due to creation of excess fluorescent background. We demonstrate creation of Ni/Si related centers showing emission in the spectral range between 767nm and 775nm and narrow line-widths of 2nm FWHM at room temperature. Measurements of the intensity auto-correlation functions prove single-photon emission. The investigated color centers can be coarsely divided into two groups: Drawing from photon statistics and the degree of polarization in excitation and emission we find that some color centers behave as two-level, single-dipole systems whereas other centers exhibit three levels and contributions from two orthogonal dipoles. In addition, some color centers feature stable and bright emission with saturation count rates up to 78kcounts/s whereas others show fluctuating count rates and three-level blinking., Comment: 7 pages, submitted to Applied Physics B, revised version

Color centers in diamond are very promising candidates among the possible realizations for practical single-photon sources because of their long-time stable emission at room temperature. The popular nitrogen-vacancy center shows single-photon emission, but within a large, phonon-broadened spectrum (~100nm), which strongly limits its applicability for quantum communication. By contrast, Ni-related centers exhibit narrow emission lines at room temperature. We present investigations on single color centers consisting of Ni and Si created by ion implantation into single crystalline IIa diamond. We use systematic variations of ion doses between 10^8/cm^2 and 10^14/cm^2 and energies between 30keV and 1.8MeV. The Ni-related centers show emission in the near infrared spectral range (~770nm to 787nm) with a small line-width (~3nm FWHM). A measurement of the intensity correlation function proves single-photon emission. Saturation measurements yield a rather high saturation count rate of 77.9 kcounts/s. Polarization dependent measurements indicate the presence of two orthogonal dipoles., Comment: 8 pages, published in conference proceedings of SPIE Photonics Europe 2010