Enhancing the measurement signal from solid state quantum sensors such as the nitrogen-vacancy (NV) center in diamond is an important problem for sensing and imaging of condensed matter systems. Here we engineer diamond scanning probes with a truncated parabolic profile that optimizes the photonic signal from single embedded NV centers, forming a high-sensitivity probe for nanoscale magnetic field imaging. We develop a scalable fabrication procedure based on dry etching with a flowable oxide mask to reliably produce a controlled tip curvature. The resulting parabolic tip shape yields a median saturation count rate of 2.1 $\pm$ 0.2 MHz, the highest reported for single NVs in scanning probes to date. Furthermore, the structures operate across the full NV photoluminescence spectrum, emitting into a numerical aperture of 0.46 and the end-facet of the truncated tip, located near the focus of the parabola, allows for small NV-sample spacings and nanoscale imaging. We demonstrate the excellent properties of these diamond scanning probes by imaging ferromagnetic stripes with a spatial resolution better than 50 nm. Our results mark a 5-fold improvement in measurement signal over the state-of-the art in scanning-probe based NV sensors.
We present an implementation of all-diamond scanning probes for scanning nitrogen-vacancy (NV) magnetometry fabricated from (111)-oriented diamond material. The realized scanning probe tips on average contain single NV spins, a quarter of which have their spin quantization axis aligned parallel to the tip direction. Such tips enable single-axis vector magnetic field imaging with nanoscale resolution, where the measurement axis is oriented normal to the scan plane. We discuss how these tips bring multiple practical advantages for NV magnetometry, in particular regarding quantitative analysis of…
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…
We describe a scanning device where a single spin is used as an ultrasensitive, nanoscale magnetic field sensor. As this "probe spin" we consider a single nitrogen-vacancy defect center in a diamond nanocrystal, attached to the tip of the scanning device. Changes in the local field seen by the probe spin are detected by optically monitoring its electron paramagnetic resonance transition. The room-temperature scanning device may be useful for performing nanoscale magnetic resonance imaging and spectroscopy, and for the characterization of magnetic nanostructures down to the single atom level.
The negatively-charged nitrogen-vacancy center (NV) in diamond forms a versatile system for quantum sensing applications. Combining the advantageous properties of this atomic-sized defect with scanning probe techniques such as atomic force microscopy (AFM) enables nanoscale imaging of e.g. magnetic fields. To form a scanning probe device, we place single NVs shallowly (i.e. < 20 nm) below the top facet of a diamond nanopillar, which is located on a thin diamond platform of typically below 1 μm thickness. This device can be attached to an AFM head, forming an excellent scanning probe tip. Furth…
Scanning probe microscopy using nitrogen vacancy (NV) centers in diamond has become a versatile tool with applications in physics, chemistry, life sciences and earth and planetary sciences. However, the fabrication of diamond scanning probes with high photon collection efficiency, NV centers with long coherence times and integrated radio frequency (RF) remains challenging due to the small physical dimensions of the probes and the complexity of the fabrication techniques. In this work, we present a simple and robust method to reliably fabricate probes that can be integrated with conventional qu…
The nitrogen-vacancy (NV) defect center in diamond has demonstrated great capability for nanoscale magnetic sensing and imaging for both static and periodically modulated target fields. However, it remains a challenge to detect and image randomly fluctuating magnetic fields. Recent theoretical and numerical works have outlined detection schemes that exploit changes in decoherence of the detector spin as a sensitive measure for fluctuating fields. Here we experimentally monitor the decoherence of a scanning NV center in order to image the fluctuating magnetic fields from paramagnetic impurities…
Nanoscale electronic transport gives rise to a number of intriguing physical phenomena that are accompanied by distinct spatial patterns of current flow. Here, we report on sensitive magnetic imaging of two-dimensional current distributions in bilayer graphene at room temperature. By combining dynamical modulation of the source-drain current with ac quantum sensing of a nitrogen-vacancy center in a diamond probe, we acquire magnetic field and current density maps with excellent sensitivities of 4.6 nT and 20 nA/$μ$m, respectively. The spatial resolution is 50-100 nm. We further introduce a set…
We present a new approach combining top down fabrication and bottom up overgrowth to create diamond photonic nanostructures in form of single-crystalline diamond nanopyramids. Our approach relies on diamond nanopillars, that are overgrown with single-crystalline diamond to form pyramidal structures oriented along crystal facets. To characterize the photonic properties of the pyramids, color centers are created in a controlled way using ion implantation and annealing. We find very high collection efficiency from color centers close to the pyramid apex. We further show excellent smoothness and s…
Spin-labeling of molecules with paramagnetic ions is an important approach for determining molecular structure, however current ensemble techniques lack the sensitivity to detect few isolated spins. In this Letter, we demonstrate two-dimensional nanoscale imaging of paramagnetic gadolinium compounds using scanning relaxometry of a single nitrogen vacancy (NV) center in diamond. Gadopentetate dimeglumine attached to an atomic force microscope tip is controllably interacted with and detected by the NV center, by virtue of the fact that the NV exhibits fast relaxation in the fluctuating magnetic …
Nitrogen-vacancy (NV) center in diamond is a promising quantum sensor with remarkably versatile sensing capabilities. While scanning NV magnetometry is well-established, NV electrometry has been so far limited to bulk diamonds. Here we demonstrate imaging external alternating (AC) and direct (DC) electric fields with a single NV at the apex of a diamond scanning tip under ambient conditions. A strong electric field screening effect is observed at low frequencies due to charge noise on the surface. We quantitatively measure its frequency dependence, and overcome this screening by mechanically o…
We report direct imaging of boundary magnetization associated with antiferromagnetic domains in magnetoelectric epitaxial Cr2O3 thin films using diamond nitrogen vacancy microscopy. We found a correlation between magnetic domain size and structural grain size which we associate with the domain formation process. We performed field cooling, i.e., cooling from above to below the Néel temperature in the presence of magnetic field, which resulted in the selection of one of the two otherwise degenerate 180 degree domains. Lifting of such a degeneracy is achievable with a magnetic field alone due to…
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 on imaging of microwave (MW) magnetic fields using a magnetometer based on the electron spin of a nitrogen vacancy center in diamond. We quantitatively image the magnetic field generated by high frequency (GHz) MW current with nanoscale resolution using a scanning probe technique. We demonstrate a MW magnetic field sensitivity in the range of a few nT/$\sqrt{\text{Hz}}$, polarization selection and broadband capabilities under ambient conditions and thereby establish the nitrogen vacancy center a versatile and high performance tool for the detection of MW fields. As a first applicatio…
We investigate bright fluorescence of nitrogen (NV)- and silicon-vacancy color centers in pyramidal, single crystal diamond tips which are commercially available as atomic force microscope probes. We coherently manipulate NV electronic spin ensembles with $T_2 = 7.7(3)\,μ$s. Color center lifetimes in different tip heights indicate effective refractive index effects and quenching. Using numerical simulations, we verify enhanced photon rates from emitters close to the pyramid apex; a situation promising for scanning probe sensing.
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…
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…
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.
Individual, luminescent point defects in solids so called color centers are atomic-sized quantum systems enabling sensing and imaging with nanoscale spatial resolution. In this overview, we introduce nanoscale sensing based on individual nitrogen vacancy (NV) centers in diamond. We discuss two central challenges of the field: First, the creation of highly-coherent, shallow NV centers less than 10 nm below the surface of single-crystal diamond. Second, the fabrication of tip-like photonic nanostructures that enable efficient fluorescence collection and can be used for scanning probe imaging bas…
We have performed low-temperature scanning tunneling spectroscopy measurements on suspended single-wall carbon nanotubes with a gate electrode allowing three-terminal spectroscopy measurements. These measurements show well-defined Coulomb diamonds as well as side peaks from phonon-assisted tunneling. The side peaks have the same gate voltage dependence as the main Coulomb peaks, directly proving that they are excitations of these states.
Optically-detected magnetic resonance using Nitrogen Vacancy (NV) color centres in diamond is a leading modality for nanoscale magnetic field imaging, as it provides single electron spin sensitivity, three-dimensional resolution better than 1 nm, and applicability to a wide range of physical and biological samples under ambient conditions. To date, however, NV-diamond magnetic imaging has been performed using real space techniques, which are either limited by optical diffraction to 250 nm resolution or require slow, point-by-point scanning for nanoscale resolution, e.g., using an atomic force …
The electrical conductivity of a material can feature subtle, nontrivial, and spatially-varying signatures with critical insight into the material's underlying physics. Here we demonstrate a conductivity imaging technique based on the atom-sized nitrogen-vacancy (NV) defect in diamond that offers local, quantitative, and noninvasive conductivity imaging with nanoscale spatial resolution. We monitor the spin relaxation rate of a single NV center in a scanning probe geometry to quantitatively image the magnetic fluctuations produced by thermal electron motion in nanopatterned metallic conductors…
The ability to probe nanoscale heat flow in a material is often limited by lack of spatial resolution. Here, we use a diamond-nanocrystal-hosted nitrogen-vacancy centre attached to the apex of a silicon thermal tip as a local temperature sensor. We apply an electrical current to heat up the tip and rely on the NV to monitor the thermal changes the tip experiences as it is brought into contact with surfaces of varying thermal conductivity. With the aid of a combined AFM/confocal setup, we image phantom microstructures with nanoscale resolution, and attain excellent agreement between the thermal…
Here, we demonstrate a gradiometry technique that significantly enhances the measurement sensitivity of such static fields, leading to new opportunities in the imaging of weakly magnetic systems. Our method relies on the mechanical oscillation of a single nitrogen-vacancy center at the tip of a scanning diamond probe, which up-converts the local spatial gradients into ac magnetic fields enabling the use of sensitive ac quantum protocols. We show that gradiometry provides important advantages over static field imaging: (i) an order-of-magnitude better sensitivity, (ii) a more localized and shar…
Planar scanning probe microscopy enables vector magnetic field imaging at the nanoscale
University of Rostock（罗斯托克大学）；Fraunhofer Institute for Applied Solid State Physics（弗劳恩霍夫应用固态物理研究所）；Walther-Meißner-Institut, Bayerische Akademie der Wissenschaften（瓦尔特-迈斯纳研究所，巴伐利亚科学院）；Technical University of Munich（慕尼黑工业大学）
We demonstrate `deterministic' launching of propagative quantum surface-plasmon polaritons at freely chosen positions on gold plasmonic receptacles. This is achieved by using as plasmon launcher a near-field scanning optical source made of a diamond nanocrystal with two Nitrogen-Vacancy color-center occupancy. Our demonstration relies on leakage-radiation microscopy of a thin homogeneous gold film and on near-field optical microscopy of a nanostructured thick gold film. Our work paves the way to future fundamental studies and applications in quantum plasmonics that require an accurate position…
Controllable atomic-scale quantum systems hold great potential as sensitive tools for nanoscale imaging and metrology. Possible applications range from nanoscale electric and magnetic field sensing to single photon microscopy, quantum information processing, and bioimaging. At the heart of such schemes is the ability to scan and accurately position a robust sensor within a few nanometers of a sample of interest, while preserving the sensor's quantum coherence and readout fidelity. These combined requirements remain a challenge for all existing approaches that rely on direct grafting of individ…
Exposure to beams of low energy electrons (2 to 30 keV) in a scanning electron microscope locally induces formation of NV-centers without thermal annealing in diamonds that have been implanted with nitrogen ions. We find that non-thermal, electron beam induced NV-formation is about four times less efficient than thermal annealing. But NV-center formation in a consecutive thermal annealing step (800C) following exposure to low energy electrons increases by a factor of up to 1.8 compared to thermal annealing alone. These observations point to reconstruction of nitrogen-vacancy complexes induced …
Leakage-radiation microscopy of a thin gold film demonstrates the ability of an ensemble of fluorescent diamond nanoparticles attached onto the apex of an optical tip to serve as an efficient near-field surface-plasmon polariton launcher. The implementation of the nanodiamond-based tip in a near-field scanning optical microscope will allow for an accurate control on the launching position, thereby opening the way to scanning plasmonics.
Arrays of NV centers in the diamond have the potential in the fields of chip-scale quantum information processing and nanoscale quantum sensing. However, determining their orientations one by one is resource intensive and time consuming. Here, in this paper, by combining scanning confocal fluorescence images and optical detected magnetic resonance, we realized a method of identifying single NV centers with the same orientation, which is practicable and high efficiency. In the proof of principle experiment, five single NV centers with the same orientation in a NV center array were identified. A…
We summarize our new scanning magnetic 3-D imaging system. This scanning system uses optically detected magnetic resonance in a single nitrogen vacancy center in a diamond nanocrystal. The theoretical analysis and the first experimental demonstrations have proved that this method has single spin sensitivity and a sub-nanoscale spatial resolution at room temperature.
The ability to perform nanoscale electric field imaging of elementary charges at ambient temperatures will have diverse interdisciplinary applications. While the nitrogen-vacancy (NV) center in diamond is capable of high-sensitivity electrometry, demonstrations have so far been limited to macroscopic field features or detection of single charges internal to diamond itself. In this work we greatly extend these capabilities by using a shallow NV center to image the electric field of a charged atomic force microscope tip with nanoscale resolution. This is achieved by measuring Stark shifts in the…
Bound states around an impurity are investigated for a two dimensional electron system in a strong magnetic field. Long-range Coulomb potential and related potentials are considered. Schrödinger equation is solved numerically to obtain the bound states. The energy and wave function of these bound states are indirectly observed by the scanning tunneling spectroscopy as local density of states (LDOS). Theoretically obtained LDOS is compared with experiment. Reasonable agreement is obtained.
Scanning diamond magnetometers based on the optically detected magnetic resonance of the nitrogen-vacancy centre offer very high sensitivity and non-invasive imaging capabilities when the stray fields emanating from ultrathin magnetic materials are sufficiently low (< 10 mT). Beyond this low-field regime, the optical signal quenches and a quantitative measurement is challenging. While the field-dependent NV photoluminescence can still provide qualitative information on magnetic morphology, this operation regime remains unexplored particularly for surface magnetisation larger than $\sim$ 3 mA. …
We demonstrate quantitative magnetic field mapping with nanoscale resolution, by applying a lock-in technique on the electron spin resonance frequency of a single nitrogen-vacancy defect placed at the apex of an atomic force microscope tip. In addition, we report an all-optical magnetic imaging technique which is sensitive to large off-axis magnetic fields, thus extending the operation range of diamond-based magnetometry. Both techniques are illustrated by using a magnetic hard disk as a test sample. Owing to the non-perturbing and quantitative nature of the magnetic probe, this work should op…
Understanding the profile of a qubit's wavefunction is key to its quantum applications. Unlike conducting systems, where a scanning tunneling microscope can be used to probe the electron distribution, there is no direct method for solid-state-defect based qubits in wide-bandgap semiconductors. In this work, we use pressure as a tuning method and a nuclear spin as an atomic scale probe to monitor the hyperfine structure of negatively charged nitrogen vacancy (NV) centers in diamonds under pressure. We present a detailed study on the nearest-neighbor $^{13}C$ hyperfine splitting in the optically…
Sub-wavelength mid-infrared imaging of locally driven photocurrents using diamond campanile probes
Lancaster University（兰卡斯特大学）；University of Nottingham（诺丁汉大学）；Shiv Nadar Institution of Eminence (Delhi-NCR)（希夫纳达尔卓越学院（德里-国家首都辖区））；Radboud University（拉德堡德大学）；Istituto Italiano di Technologia（意大利理工学院）
Magnetic microscopy of malarial hemozoin nanocrystals was performed using optically detected magnetic resonance imaging of near-surface diamond nitrogen-vacancy centers. Hemozoin crystals were extracted from $Plasmodium$-$falciparum$-infected human blood cells and studied alongside synthetic hemozoin crystals. The stray magnetic fields produced by individual crystals were imaged at room temperature as a function of applied field up to 350 mT. More than 100 nanocrystals were analyzed, revealing the distribution of their magnetic properties. Most crystals ($96\%$) exhibit a linear dependence of …
Scanning probe microscopy is one of the most versatile windows into the nanoworld, providing imaging access to a variety of sample properties, depending on the probe employed. Tunneling probes map electronic properties of samples, magnetic and photonic probes image their magnetic and dielectric structure while sharp tips probe mechanical properties like surface topography, friction or stiffness. Most of these observables, however, are accessible only under limited circumstances. For instance, electronic properties are measurable only on conducting samples while atomic-resolution force microsco…
The Dzyaloshinskii-Moriya Interaction (DMI) has recently attracted considerable interest owing to its fundamental role in the stabilization of chiral spin textures in ultrathin ferromagnets, which are interesting candidates for future spintronic technologies. Here we employ a scanning nano-magnetometer based on a single nitrogen-vacancy (NV) defect in diamond to locally probe the strength of the interfacial DMI in CoFeB/MgO ultrathin films grown on different heavy metal underlayers X=Ta,TaN, and W. By measuring the stray field emanating from DWs in micron-long wires of such materials, we obser…
To study the magnetic dynamics of superparamagnetic nanoparticles we use scanning probe relaxometry and dephasing of the nitrogen-vacancy (NV) center in diamond, characterizing the spin-noise of a single 10-nm magnetite particle. Additionally, we show the anisotropy of the NV sensitivity's dependence on the applied decoherence measurement method. By comparing the change in relaxation (T 1 ) and dephasing (T 2 ) time in the NV center when scanning a nanoparticle over it, we are able to extract the nanoparticle's diameter and distance from the NV center using an Ornstein-Uhlenbeck model for the …
The spatial resolution of imaging magnetometers has benefited from scanning probe techniques. The requirement that the sample perturbs the scanning probe through a magnetic field external to its volume limits magnetometry to samples with pre-existing magnetization. We propose a magnetometer in which the perturbation is reversed: the probe's magnetic field generates a response of the sample, which acts back on the probe and changes its energy. For an NV$^-$ spin center in diamond this perturbation changes the fine-structure splitting of the spin ground state. Sensitive measurement techniques us…
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…
Magnetometry and magnetic imaging with nitrogen-vacancy (NV) defects in diamond rely on the optical detection of electron spin resonance (ESR). However, this technique is inherently limited to magnetic fields that are weak enough to avoid electron spin mixing. Here we focus on the high off-axis magnetic field regime for which spin mixing alters the NV defect spin dynamics. We first study in a quantitative manner the dependence of the NV defect optical properties on the magnetic field vector B. Magnetic-field-dependent time-resolved photoluminescence (PL) measurements are compared to a seven-le…
Strong spin-orbit interaction characteristic for p-type GaAs systems, makes such systems promising for the realization of spintronic devices. Here we report on transport measurements in nanostructures fabricated on p-type, C-doped GaAs heterostructures by scanning probe oxidation lithography. We observe conductance quantization in a quantum point contact, as well as pronounced Coulomb resonances in two quantum dots with different geometries. Charging energies for both dots, extracted from Coulomb diamond measurements are in agreement with the lithographic dimensions of the dots. The absence of…
Quantum control of individual spins in condensed matter systems is an emerging field with wide-ranging applications in spintronics, quantum computation, and sensitive magnetometry. Recent experiments have demonstrated the ability to address and manipulate single electron spins through either optical or electrical techniques. However, it is a challenge to extend individual spin control to nanoscale multi-electron systems, as individual spins are often irresolvable with existing methods. Here we demonstrate that coherent individual spin control can be achieved with few-nm resolution for proximal…
We present a novel spectroscopy protocol based on optimal control of a single quantum system. It enables measurements with quantum-limited sensitivity (η_ω~ 1/sqrt(T_2^*),T_2^* denoting the system's coherence time) but has an orders of magnitude larger dynamic range than pulsed spectroscopy methods previously employed for this task. We employ this protocol to image nanoscale magnetic fields with a single scanning NV center in diamond. Here, our scheme enables quantitative imaging of a strongly inhomogeneous field in a single scan without closed-loop control, which has previously been necessary…
Quantum sensors based on solid-state spins provide tremendous opportunities in a wide range of fields from basic physics and chemistry to biomedical imaging. However, integrating them into a scanning probe microscope to enable practical, nanoscale quantum imaging is a highly challenging task. Recently, the use of single spins in diamond in conjunction with atomic force microscopy techniques has allowed significant progress towards this goal, but generalisation of this approach has so far been impeded by long acquisition times or by the absence of simultaneous topographic information. Here we r…
The recent observation of current-induced domain wall (DW) motion with large velocity in ultrathin magnetic wires has opened new opportunities for spintronic devices. However, there is still no consensus on the underlying mechanisms of DW motion. Key to this debate is the DW structure, which can be of Bloch or Néel type, and dramatically affects the efficiency of the different proposed mechanisms. To date, most experiments aiming to address this question have relied on deducing the DW structure and chirality from its motion under additional in-plane applied fields, which is indirect and involv…
Magnetic sensing and imaging instruments are important tools in biological and material sciences. There is an increasing demand for attaining higher sensitivity and spatial resolution, with implementations using a single qubit offering potential improvements in both directions. In this article we describe a scanning magnetometer based on the nitrogen-vacancy center in diamond as the sensor. By means of a quantum-assisted readout scheme together with advances in photon collection efficiency, our device exhibits an enhancement in signal to noise ratio of close to an order of magnitude compared t…
Nanoscale Dipolar Fields in Artificial Spin Ice Probed by Scanning NV Magnetometry
RPTU University Kaiserslautern-Landau, Department of Physics and State Research Center OPTIMAS（凯泽斯劳滕-兰道工业大学物理系及OPTIMAS州立研究中心）；Thomas J. Watson College of Engineering and Applied Science, Binghamton University（宾汉姆顿大学托马斯·J·沃森工程与应用科学学院）；Department of Physics & Astronomy, University of Delaware（特拉华大学物理与天文学系）
