Exchange interactions between isolated pairs of spin centers in diamond have been calculated, based on an accurate atomistic electronic structure for diamond and any impurity atoms, for spin-center separations up to 2~nm. The exchange interactions exceed dipolar interactions for spin center separations less than 3~nm. NV$^-$ spin centers, which are extended defects, interact very differently depending on the relative orientations of the symmetry axis of the spin center and the radius vector connecting the pair. Exchange interactions between transition-metal dopants behave similarly to those of NV$^-$ centers. The Mn\---Mn exchange interaction decays with a much longer length scale than the Cr\---Cr and Ni\---Ni exchange interactions, exceeding dipolar interactions for Mn\---Mn separations less than 5~nm. Calculations of these highly anisotropic and spin-center-dependent interactions provide the potential for design of the spin-spin interactions for novel nanomagnetic structures.
Coulomb diamonds are the archetypal signatures of Coulomb blockade, a well-known charging effect mainly observed in nanometer-sized "electronic islands" tunnel-coupled with charge reservoirs. Here, we identify apparent Coulomb diamond features in the scanning gate spectroscopy of a quantum point contact carved out of a semiconductor heterostructure, in the quantum Hall regime. Varying the scanning gate parameters and the magnetic field, the diamonds are found to smoothly evolve to checkerboard patterns. To explain this surprising behavior, we put forward a model which relies on the presence of…
We present nanoscale NMR measurements performed with nitrogen-vacancy (NV) centers located down to about 2 nm from the diamond surface. NV centers were created by shallow ion implantation followed by a slow, nanometer-by-nanometer removal of diamond material using oxidative etching in air. The close proximity of NV centers to the surface yielded large 1H NMR signals of up to 3.4 uT-rms, corresponding to ~330 statistically polarized or ~10 fully polarized proton spins in a ~(1.8 nm)^3 detection volume.
Magnetic resonance imaging (MRI) has revolutionized biomedical science by providing non-invasive, three-dimensional biological imaging. However, spatial resolution in conventional MRI systems is limited to tens of microns, which is insufficient for imaging on molecular and atomic scales. Here we demonstrate an MRI technique that provides sub-nanometer spatial resolution in three dimensions, with single electron-spin sensitivity. Our imaging method works under ambient conditions and can measure ubiquitous 'dark' spins, which constitute nearly all spin targets of interest and cannot otherwise be…
Sensitive probing of temperature variations on nanometer scales represents an outstanding challenge in many areas of modern science and technology. In particular, a thermometer capable of sub-degree temperature resolution as well as integration within a living system could provide a powerful new tool for many areas of biological research, including temperature-induced control of gene expression and cell-selective treatment of disease. Here, we demonstrate a new approach to nanoscale thermometry that utilizes coherent manipulation of the electronic spin associated with nitrogen-vacancy (NV) col…
Atomic-size spin defects in solids are unique quantum systems. Most applications require nanometer positioning accuracy, which is typically achieved by low energy ion implantation. So far, a drawback of this technique is the significant residual implantation-induced damage to the lattice, which strongly degrades the performance of spins in quantum applications. In this letter we show that the charge state of implantation-induced defects drastically influences the formation of lattice defects during thermal annealing. We demonstrate that charging of vacancies localized at e.g. individual nitrog…
Measuring local temperature with a spatial resolution on the order of a few nanometers has a wide range of applications from semiconductor industry over material to life sciences. When combined with precision temperature measurement it promises to give excess to small temperature changes caused e.g. by chemical reactions or biochemical processes. However, nanoscale temperature measurements and precision have excluded each other so far owing to the physical processes used for temperature measurement of limited stability of nanoscale probes. Here we experimentally demonstrate a novel nanoscale t…
We investigate spin and optical properties of individual nitrogen-vacancy centers located within 1-10 nm from the diamond surface. We observe stable defects with a characteristic optically detected magnetic resonance spectrum down to lowest depth. We also find a small, but systematic spectral broadening for defects shallower than about 2 nm. This broadening is consistent with the presence of a surface paramagnetic impurity layer [Tisler et al., ACS Nano 3, 1959 (2009)] largely decoupled by motional averaging. The observation of stable and well-behaved defects very close to the surface is criti…
Magnetic imaging using color centers in diamond through both scanning and wide-field methods offers a combination of unique capabilities for studying superconductivity, for example, enabling accurate vector magnetometry at high temperature or high pressure, with spatial resolution down to the nanometer scale. The paper briefly reviews various experimental modalities in this rapidly developing nascent field and provides an outlook towards possible future directions.
We demonstrate a method of magnetic resonance imaging with single nuclear-spin sensitivity under ambient conditions. It employs a network of isolated electronic-spin quantum bits (qubits) that act as quantum reporters on the surface of high purity diamond. The reporter spins are localized with nanometer-scale uncertainty, and their quantum state is coherently manipulated and measured optically via a proximal nitrogen-vacancy (NV) color center located a few nanometers below the diamond surface. The quantum reporter network is then used for sensing, coherent coupling and imaging individual proto…
Spin waves in ferrimagnetic yttrium iron garnet (YIG) films with ultralow magnetic damping are relevant for magnon-based spintronics and low-power wave-like computing. The excitation frequency of spin waves in YIG is rather low in weak external magnetic fields because of its small saturation magnetization, which limits the potential of YIG films for high-frequency applications. Here, we demonstrate how exchange-coupling to a CoFeB film enables efficient excitation of high-frequency perpendicular standing spin waves (PSSWs) in nanometer-thick (80 nm and 295 nm) YIG films using uniform microwave…
The electronic spin of the nitrogen vacancy (NV) center in diamond forms an atomically sized, highly sensitive sensor for magnetic fields. To harness the full potential of individual NV centers for sensing with high sensitivity and nanoscale spatial resolution, NV centers have to be incorporated into scanning probe structures enabling controlled scanning in close proximity to the sample surface. Here, we present an optimized procedure to fabricate single-crystal, all-diamond scanning probes starting from commercially available diamond and show a highly efficient and robust approach for integra…
The distributions of magnetization orientation for both Landau and diamond domain structures in nano-rectangles have been investigated by micromagnetic simulation with various exchange coefficient and anisotropy constant. Both symmetric and asymmetric magnetization splitting are found in diamond domain structure, as well as only symmetric magnetization splitting in Landau structure. In the Landau structure, the splitting angle increases with the exchange coefficient but decreases slightly with the anisotropy constant, suggesting that the exchange interaction mainly contributes to the magnetiza…
We measure diffusion of organic molecules located a few nanometers from the diamond surface. To study molecular diffusion, we perform local detection of nuclear magnetic resonance, based on single shallow Nitrogen-Vacancy (NV) centers in diamond. Specifically, we demonstrate measurements of translational diffusion coefficient of phospholipids in an artificial cell membrane by employing correlation spectroscopy. An analysis of correlation decay curves using different diffusion models shows, that a simple 2D diffusion model gives satisfactory diffusion coefficients, although the choice of the mo…
Despite decades of advances in magnetic imaging, obtaining direct, quantitative information with nanometer scale spatial resolution remains an outstanding challenge. Recently, a new technique has emerged that employs a single nitrogen-vacancy (NV) defect in diamond as an atomic-size magnetometer. Although NV magnetometry promises significant advances in magnetic imaging, the effectiveness of the technique, when applied to realistic magnetic nanostructures, remains to be demonstrated. Here we use a scanning NV magnetometer to image a magnetic vortex, which is one of the most iconic object of na…
We report on the fabrication and characterization of a Fabry-Perot microcavity enclosing a thin diamond membrane at cryogenic temperatures. The cavity is designed to enhance resonant emission of single nitrogen-vacancy centers by allowing spectral and spatial tuning while preserving the optical properties observed in bulk diamond. We demonstrate cavity finesse at cryogenic temperatures within the range of F = 4,000-12,000 and find a sub-nanometer cavity stability. Modeling shows that coupling nitrogen-vacancy centers to these cavities could lead to an increase of remote entanglement success ra…
We present two applications of a single nitrogen vacancy center in a nanodiamond as quantum probe for plasmonic nanostructures. Coupling to the nanostructures is achieved in a highly controlled manner by picking up a pre-characterized nanocrystal with an atomic force microscope and placing it at the desired position. Local launching of single excitations into a nanowire with a spatial control of few nanometers is demonstrated. Further, a two dimensional map of the electromagnetic environment of a plasmonic bowtie antenna was derived, resembling an ultimate limit of fluorescence lifetime nanosc…
Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal…
We report on the noise spectrum experienced by few nanometer deep nitrogen-vacancy centers in diamond as a function of depth, surface coating, magnetic field and temperature. Analysis reveals a double-Lorentzian noise spectra consistent with a surface electronic spin bath, with slower dynamics due to spin-spin interactions and faster dynamics related to phononic coupling. These results shed new light on the mechanisms responsible for surface noise affecting shallow spins at semiconductor interfaces, and suggests possible directions for further studies. We demonstrate dynamical decoupling from …
We demonstrate nanometer-precision depth control of nitrogen-vacancy (NV) center creation near the surface of synthetic diamond using an in situ nitrogen delta-doping technique during plasma-enhanced chemical vapor deposition. Despite their proximity to the surface, doped NV centers with depths (d) ranging from 5 - 100 nm display long spin coherence times, T2 > 100 \mus at d = 5 nm and T2 > 600 \mus at d \geq 50 nm. The consistently long spin coherence observed in such shallow NV centers enables applications such as atomic-scale external spin sensing and hybrid quantum architectures.
The negatively-charged nitrogen-vacancy (NV) center in diamond has been shown recently as an excellent sensor for external spins. Nevertheless, their optimum engineering in the near-surface region still requires quantitative knowledge in regard to their activation by vacancy capture during thermal annealing. To this aim, we report on the depth profiles of near-surface helium-induced NV centers (and related helium defects) by step-etching with nanometer resolution. This provides insights into the efficiency of vacancy diffusion and recombination paths concurrent to the formation of NV centers. …
Understanding the dynamics of molecules adsorbed to surfaces or confined to small volumes is a matter of increasing scientific and technological importance. Here, we demonstrate a pulse protocol using individual paramagnetic nitrogen vacancy (NV) centers in diamond to observe the time evolution of 1H spins from organic molecules located a few nanometers from the diamond surface. The protocol records temporal correlations among the interacting 1H spins, and thus is sensitive to the local system dynamics via its impact on the nuclear spin relaxation and interaction with the NV. We are able to ga…
We propose a multilayer device comprising of a thin-film-based ferromagnetic hetero-structure (FMH) deposited on a diamond layer doped with nitrogen vacancy centers (NVC's). We find that when the NVC's are in close proximity (1-2 nm) with the FMH, the exchange energy is comparable to, and may even surpass the magnetostatic interaction energy. This calls for the need to consider and utilize both effects in magnetometry based on NVC's in diamond. As the distance between the FMH and NVC is decreased to the sub-nanometer scale, the exponential increase in the exchange energy suggests spintronic ap…
We show that the positioning of a nanometer length scale dielectric object, such as a diamond nanocrystal, in the vicinity of a gold bowtie nanoantenna can be used to tune the plasmonic mode spectrum on the order of a linewidth. We further show that the intrinsic luminescence of gold enhanced in the presence of nanometer-scale roughness couples efficiently to the plasmon mode and carries the same polarization anisotropy. Our findings have direct implications for cavity quantum electrodynamics related applications of hybrid antenna-emitter complexes.
Shallow, negatively-charged Nitrogen-Vacancy centers (NV-) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV0 centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm2). Raman spectroscopy, optically-detected-magnetic-resonance (ODMR) and charge-photoconversion fluorescence…
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 …
Single-molecule nuclear magnetic resonance (NMR) is a crown-jewel challenge in the field of magnetic resonance spectroscopy and has important applications in chemical analysis and in quantum computing. Recently, it becomes possible to tackle this grand challenge thanks to experimental advances in preserving quantum coherence of nitrogen-vacancy (NV) center spins in diamond as a sensitive probe and theoretical proposals on atomic-scale magnetometry via dynamical decoupling control. Through decoherence measurement of NV centers under dynamical decoupling control, sensing of single $^{13}\textbf{…
Controlling the magnetic ground states at the nanoscale is a long-standing basic research problem and an important issue in magnetic storage technologies. Here, we designed a nanostructured material that exhibits very unusual hysteresis loops due to a transition between vortex and double pole states. Arrays of 700 nm diamond-shape nanodots consisting of Py(30 nm)/Ru(tRu)/Py(30 nm) (Py, permalloy (Ni80Fe20)) trilayers were fabricated by interference lithography and e-beam evaporation. We show that varying the Ru interlayer spacer thickness (tRu) governs the interaction between the Py layers. We…
The nitrogen-vacancy (NV) centre, as a promising candidate solid state system of quantum information processing, its electron spin coherence is influenced by the magnetic field fluctuations due to the local environment. In pure diamonds, the environment consists of hundreds of C-13 nuclear spins randomly spreading in several nanometers range forming a spin bath. Controlling and prolonging the electron spin coherence under the influence of spin bath are challenging tasks for the quantum information processing. On the other hand, for a given bath distribution, many of its characters are encoded …
Transition-metal interfaces and multilayers are a very promising class of systems to realize nanometer-sized, stable magnetic skyrmions for future spintronic devices. For room temperature applications it is crucial to understand the interactions which control the stability of isolated skyrmions. Typically, skyrmion properties are explained by the interplay of pair-wise exchange interactions, the Dzyaloshinskii-Moriya interaction and the magnetocrystalline anisotropy energy. Here, we demonstrate that higher-order exchange interactions -- which have so far been neglected -- can play a key role f…
An obstacle for spin-based quantum sensors is magnetic noise due to proximal spins. However, such a spin cluster surrounding the sensor can become an asset, if it can be controlled. Here, we polarize and readout a cluster of three nitrogen (N) electron spins coupled to a single nitrogen-vacancy (NV) spin in diamond. We further achieve sub-nm localization of the cluster spins. Finally, we demonstrate coherent spin exchange between the species by simultaneous dressing of the NV and the N states. These results establish the feasibility of environment-assisted sensing and quantum simulations with …
The production of correlated Stokes (S) and anti-Stokes (aS) photons (SaS process) mediated by real or virtual phonon exchange has been reported in many transparent materials. In this work, we investigate the polarization and time correlations of SaS photon pairs produced in a diamond sample. We demonstrate that both S and aS photons have mainly the same polarization of the excitation laser. We also perform a pump-and-probe experiment to measure the decay rate of the SaS pair production, evidencing the fundamental diference between the real and virtual (phonon exchange) processes. In real proc…
The realization of scalable arrangements of nitrogen vacancy (NV) centers in diamond remains a key challenge on the way towards efficient quantum information processing, quantum simulation and quantum sensing applications. Although technologies based on implanting NV-center in bulk diamond crystals or hybrid device approaches have been developed, they are limited in the achievable spatial resolution and by the intricate technological complexities involved in achieving scalability. We propose and demonstrate a novel approach for creating an arrangement of NV-centers, based on the self-assemblin…
Electron-spin nitrogen-vacancy color centers in diamond are a natural candidate to act as a quantum memory for superconducting qubits because of their large collective coupling and long coherence times. We report here the first demonstration of strong coupling and coherent exchange of a single quantum of energy between a flux-qubit and an ensemble of nitrogen-vacancy color centers.
We present a scheme of positioning a single electron spin with sub-nanometer resolution through multiple nitrogen-vacancy centers in diamond. With unwanted noise suppressed by dynamical decoupling, the spin coherence of each center develops characteristic oscillations due to a single electron spin located $4{\sim20}$ nm away from the centers. We can extract the position information from the characteristic electron spin-coherence oscillations of each center. This scheme is useful for high-resolution nanoscale magnetometry and spin-based quantum computing.
The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridge the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter triggered by the impulsive optical generation of spin excitations with the shortest possible nanometer-wavelength and femtosecond-period. Our experiments also disclose a p…
We present a novel approach to spin manipulation in atomic-scale nanostructures. Our ab initio calculations clearly demonstrate that it is possible to tune magnetic properties of sub-nanometer structures by adjusting the geometry of the system. By the example of two surface-based systems we demonstrate that (i) the magnetic moment of a single adatom coupled to a buried magnetic Co layer can be stabilized in either a ferromagnetic or an antiferromagnetic configuration depending on the spacer thickness. It is found that a buried Co layer has a profound effect on the exchange interaction between …
We demonstrate high resolution scanning fluorescence resonance energy transfer 10 microscopy between a single nitrogen-vacancy center as donor and graphene as acceptor. 11 Images with few nanometer resolution of single and multilayer graphene structures were 12 attained. An energy transfer efficiency of 30% at distances of 10nm between a single 13 defect and graphene was measured. Further the energy transfer distance dependence of 14 the nitrogen-vacancy center to graphene was measured to show the predicted d-4 15 dependence. Our studies pave the way towards a diamond defect center based versa…
Defect centers in diamond are exceptional solid-state quantum systems that can have exceedingly long electron and nuclear spin coherence times. So far, single-qubit gates for the nitrogen nuclear spin, a two-qubit gate with a nitrogen-vacancy (NV) center electron spin, and entanglement between nearby nitrogen nuclear spins have been demonstrated. Here, we develop a scheme to implement a universal two-qubit gate between two distant nitrogen nuclear spins. Virtual excitation of an NV center that is embedded in an optical cavity can scatter a laser photon into the cavity mode; we show that this p…
Electron spins in solids constitute remarkable quantum sensors. Individual defect centers in diamond were used to detect individual nuclear spins with nanometer scale resolution, and ensemble magnetometers rival SQUID and vapor cell magnetometers when taking into account room temperature operation and size. NV center spins can also detect electric field vectors, despite their weak coupling to electric fields. %even that of an isolated fundamental charge, despite their weak coupling to electric fields. Here, we employ ensembles of NV center spins to measure macroscopic AC electric vector fields…
Nitrogen vacancy (NV) color centers in diamond have emerged as highly versatile optical emitters that exhibit room temperature spin properties. These characteristics make NV centers ideal for magnetometry, which plays an important role in chemical and biological sensing applications. The integration of NV magnetometers with microfluidic systems could enable the study of isolated chemical and biological samples in a fluid environment with high spatial resolution. Here we demonstrate a method to perform localized magnetometry with nanometer spatial precision using a single NV center in a microfl…
We report a study of the magnetic field dependence of the photo-luminescence of NV$^-$ centers (negatively charged nitrogen-vacancy centers) in diamond single crystals. In such a magnetic field dependence characteristic lines are observed, which are coming from Level Anti-Crossings (LACs) in the coupled electron-nuclear spin system. For enhancing the sensitivity, we used lock-in detection to measure the photo-luminescence intensity and observed a remarkably strong dependence of the LAC-derived lines on the modulation frequency. Upon decreasing of the modulation frequency from 12 kHz to 17 Hz t…
The negatively-charged NV$^-$-center in diamond has shown great success in nanoscale, high-sensitivity magnetometry. Efficient fluorescence detection is crucial for improving the sensitivity. Furthermore, integrated devices enable practicable sensors. Here, we present a novel architecture which allows us to create NV$^-$-centers a few nanometers below the diamond surface, and at the same time in the mode field maximum of femtosecond-laser-written type-II waveguides. We experimentally verify the coupling efficiency, showcase the detection of magnetic resonance signals through the waveguides and…
The nitrogen-vacancy (NV) center in diamond has been extensively studied in recent years for its remarkable quantum coherence properties that make it an ideal candidate for room temperature quantum computing and quantum sensing schemes. However, these schemes rely on spin-spin dipolar interactions, which require the NV centers to be within a few nanometers from each other while still separately addressable, or to be in close proximity of the diamond surface, where their coherence properties significantly degrade. Here we demonstrate a method for overcoming these limitations using a hybrid yttr…
