A single nitrogen-vacancy (NV) center in diamond is a prime candidate for a solid-state quantum magnetometer capable of detecting single nuclear spins with prospective application to nuclear magnetic resonance (NMR) at the nanoscale. Nonetheless, an NV magnetometer is still less accessible to many chemists and biologists, as its experimental setup and operational principle are starkly different from those of conventional NMR. Here, we design, construct, and operate a compact tabletop-sized system for quantum sensing with a single NV center, built primarily from commercially available optical components and electronics. We show that our setup can implement state-of-the-art quantum sensing protocols that enable the detection of single $^{13}$C nuclear spins in diamond and the characterization of their interaction parameters, as well as the detection of a small ensemble of proton nuclear spins on the diamond surface. This article providing extensive discussions on the details of the setup and the experimental procedures, our system will be reproducible by those who have not worked on the NV centers previously.
We demonstrate real-time magnetometry by detecting fluorescence from a nitrogen vacancy center in the setting of coherent population trapping and by estimating magnetic field from the time series of the observed photon counts, which are correlated with the underlying field. The proof-of-principle experiment uses an external time-varying magnetic field that follows an Ornstein-Uhlenbeck (OU) process. By taking into consideration the statistical properties of the OU process, a Bayesian inference-based estimator can effectively update dynamical information of the field in real time with the detec…
We discuss multipulse magnetometry that exploits all three magnetic sublevels of the S=1 nitrogen-vacancy center in diamond to achieve enhanced magnetic field sensitivity. Based on dual frequency microwave pulsing, the scheme works in arbitrary magnetic bias fields and is twice as sensitive to ac magnetic fields as conventional two-level magnetometry. We derive the spin evolution operator for dual frequency microwave excitation and show its effectiveness for double-quantum state swaps. Using multipulse sequences of up to 128 pulses under optimized conditions, we show enhancement of the SNR by …
We demonstrate a spectrum demodulation technique for greatly speeding up the data acquisition rate in scanning nitrogen-vacancy center magnetometry. Our method relies on a periodic excitation of the electron spin resonance by fast, wide-band frequency sweeps combined with a phase-locked detection of the photo-luminescence signal. The method can be extended by a frequency feedback to realize real-time tracking of the spin resonance. Fast scanning magnetometry is especially useful for samples where the signal dynamic range is large, of order millitesla, like for ferro- or ferrimagnets. We demons…
Shallow nitrogen-vacancy (NV) centers in diamond are promising for nano-magnetometry for they can be placed proximate to targets. To study the intrinsic magnetic properties, zero-field magnetometry is desirable. However, for shallow NV centers under zero field, the strain near diamond surfaces would cause level anti-crossing between the spin states, leading to clock transitions whose frequencies are insensitive to magnetic signals. Furthermore, the charge noises from the surfaces would induce extra spin decoherence and hence reduce the magnetic sensitivity. Here we demonstrate that the relativ…
We report on the use of a single NV center to probe fluctuating AC magnetic fields. Using engineered currents to induce random changes in the field amplitude and phase, we show that stochastic fluctuations reduce the NV center sensitivity and, in general, make the NV response field-dependent. We also introduce two modalities to determine the field spectral composition, unknown a priori in a practical application. One strategy capitalizes on the generation of AC-field-induced coherence 'revivals', while the other approach uses the time-tagged fluorescence intensity record from successive NV obs…
Nitrogen-vacancy (NV) centers in diamond are suitable sensors of high-sensitivity magnetometry which have attracted much interest in recent years. Here, we demonstrate sensitivity-enhanced ensembles magnetometry via adaptively complete transitions overlapping with a bias magnetic field equally projecting onto all existing NV orientations. Under such conditions, the spin transitions corresponding to different NV orientations are completely overlapped which will bring about an obviously improved photoluminescence contrast. And we further introduce particle swarm optimization into the calibration…
We demonstrate an absolute magnetometer immune to temperature fluctuation and strain inhomogeneity, based on quantum beats in the ground state of nitrogen-vacancy centers in diamond. We apply this technique to measure low-frequency magnetic field noise using a single nitrogen-vacancy center located within 500 nm of the surface of an isotopically-pure (99.99% C12) diamond. The photon-shot-noise limited sensitivity achieves 38 nT/Hz^1/2 for 4.45 s acquisition time, a factor of 2^1/2 better than the implementation which uses only two spin levels. For long acquisition times (>10 s), we realize up …
Spatially resolved quantum magnetometry and stray-field reconstruction of permalloy microdisks using boron-vacancy centers in hexagonal boron nitride
Helmholtz-Zentrum Dresden-Rossendorf（德累斯顿罗森多夫亥姆霍兹中心）；Technische Universität Dresden（德累斯顿工业大学）；Leibniz Institute for Solid State and Materials Research（莱布尼茨固体与材料研究所）；National Institute for Materials Science（国家物质材料研究所）
Ensembles of nitrogen-vacancy centers in diamond are a highly promising platform for high-sensitivity magnetometry, whose efficacy is often based on efficiently generating and monitoring magnetic-field dependent infrared fluorescence. Here we report on an increased sensing efficiency with the use of a 532-nm resonant confocal cavity and a microwave resonator antenna for measuring the local magnetic noise density using the intrinsic nitrogen-vacancy concentration of a chemical-vapor deposited single-crystal diamond. We measure a near-shot-noise-limited magnetic noise floor of 200 pT/$\sqrt{\tex…
Detection of AC magnetic fields at the nanoscale is critical in applications ranging from fundamental physics to materials science. Isolated quantum spin defects, such as the nitrogen-vacancy center in diamond, can achieve the desired spatial resolution with high sensitivity. Still, vector AC magnetometry currently relies on using different orientations of an ensemble of sensors, with degraded spatial resolution, and a protocol based on a single NV is lacking. Here we propose and experimentally demonstrate a protocol that exploits a single NV to reconstruct the vectorial components of an AC ma…
We report on the implementation of a scanning nitrogen-vacancy (NV) magnetometer in a dry dilution refrigerator. Using pulsed optically detected magnetic resonance combined with efficient microwave delivery through a co-planar waveguide, we reach a base temperature of 350 mK, limited by experimental heat load and thermalization of the probe. We demonstrate scanning NV magnetometry by imaging superconducting vortices in a 50-nm-thin aluminum microstructure. The sensitivity of our measurements is approximately 3 μT per square root Hz. Our work demonstrates the feasibility for performing non-inva…
We demonstrate a robust, scale-factor-free vector magnetometer, which uses a closed-loop frequency-locking scheme to simultaneously track Zeeman-split resonance pairs of nitrogen-vacancy (NV) centers in diamond. Compared with open-loop methodologies, this technique is robust against fluctuations in temperature, resonance linewidth, and contrast; offers a three-order-of-magnitude increase in dynamic range; and allows for simultaneous interrogation of multiple transition frequencies. By directly detecting the resonance frequencies of NV centers aligned along each of the diamond's four tetrahedra…
We demonstrate magnetometry by detection of the spin state of high-density nitrogen-vacancy ensembles in diamond using optical absorption at 1042 nm. With this technique, measurement contrast, and collection efficiency can approach unity, leading to an increase in magnetic sensitivity compared to the more common method of collecting red fluorescence. Working at 75 K with a sensor with effective volume $50 \times 50 \times 300$ microns^3, we project photon shot-noise limited sensitivity of 5 pT in one second of acquisition and bandwidth from dc to a few megahertz. Operation in a gradiometer con…
This article proposes a scheme for nitrogen-vacancy (NV) center magnetometry that combines the advantages of lock-in detection and pulse-type scheme. The optimal conditions, optimal sensitivity, and noise-suppression capability of the proposed method are compared with those of the conventional methods from both theoretical and simulation points of view. Through experimental measurements, a four-time improvement in sensitivity and 60-times improvement in minimum resolvable magnetic field (MRMF) was obtained. By using a confocal experiment setup, proposed scheme achieves a sensitivity of 3 nT/Hz…
We demonstrate magnetic field sensing using an ensemble of nitrogen-vacancy centers by recording the variation in the pump-light absorption due to the spin-polarization dependence of the total ground state population. Using a 532 nm pump laser, we measure the absorption of native nitrogen-vacancy centers in a chemical vapor deposited diamond placed in a resonant optical cavity. For a laser pump power of 0.4 W and a cavity finesse of 45, we obtain a noise floor of $\sim$ 100 nT/$\sqrt{\textrm{Hz}}$ spanning a bandwidth up to 125 Hz. We project a photon shot-noise-limited sensitivity of $\sim$ 1…
Master equation-based model for infrared-based magnetometry with nitrogen-vacancy centers in diamond cavities: a path to sub-picotesla sensitivity at sub-millimeter scales
Magnetometry with nitrogen-vacancy color centers in diamond has gained significant interest among researchers in recent years. Absolute knowledge of the three-dimensional orientation of the magnetic field is necessary for many applications. Conventional magnetometry measurements are usually performed with NV ensembles in a bulk diamond with a thin NV layer or a scanning probe in the form of a diamond tip, which requires a smooth sample surface and proximity of the probing device, often limiting the sensing capabilities. Here, we present a method for determining the three-dimensional orientatio…
Silicon Carbide is a promising host material for spin defect based quantum sensors owing to its commercial availability and established techniques for electrical and optical microfabricated device integration. The negatively charged silicon vacancy is one of the leading spin defects studied in silicon carbide owing to its near telecom photoemission, high spin number, and nearly temperature independent ground state zero field splitting. We report the realization of nanoTesla shot-noise limited ensemble magnetometry based on optically detected magnetic resonance with the silicon vacancy in 4H si…
Ensembles of nitrogen-vacancy (NV) centers in diamonds are widely utilized for magnetometry, magnetic-field imaging and magnetic-resonance detection. They have not been used for magnetometry at zero ambient field because Zeeman sublevels lose first-order sensitivity to magnetic fields as they are mixed due to crystal strain or electric fields. In this work, we realize a zero-field (ZF) magnetometer using polarization-selective microwave excitation in a 12C-enriched HPHT crystal sample. We employ circularly polarized microwaves to address specific transitions in the optically detected magnetic …
The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen-vacancy centre in diamond - a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen-vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of …
Scanning magnetometry with nitrogen-vacancy (NV) centers in diamond has emerged as a powerful microscopy for studying weak stray field patterns with nanometer resolution. Due to the internal crystal anisotropy of the spin defect, however, external bias fields -- critical for the study of magnetic materials -- must be applied along specific spatial directions. In particular, the most common diamond probes made from {100}-cut diamond only support fields at an angle of $θ= 55^\circ$ from the surface normal. In this paper, we report fabrication of scanning diamond probes from {110}-cut diamond whe…
We report a new method to determine the orientation of individual nitrogen-vacancy (NV) centers in a bulk diamond and use them to realize a calibration-free vector magnetometer with nanoscale resolution. Optical vortex beam is used for optical excitation and scanning the NV center in a [111]-oriented diamond. The scanning fluorescence patterns of NV center with different orientations are completely different. Thus, the orientation information on each NV center in the lattice can be known directly without any calibration process. Further, we use three differently oriented NV centers to form a m…
We demonstrate a cavity-enhanced room-temperature magnetic field sensor based on nitrogen-vacancy centers in diamond. Magnetic resonance is detected using absorption of light resonant with the 1042 nm spin-singlet transition. The diamond is placed in an external optical cavity to enhance the absorption, and significant absorption is observed even at room temperature. We demonstrate a magnetic field sensitivity of 2.5 nT/sqrt(Hz), and project a photon shot-noise-limited sensitivity of 70 pT/sqrt(Hz) for a few mW of infrared light, and a quantum projection-noise-limited sensitivity of 250 fT/sqr…
We propose a high-sensitivity magnetometry scheme based on a diamond Raman laser with visible pump absorption by an ensemble of coherently microwave driven negatively charged nitrogen-vacancy centres (NV) in the same diamond crystal. The NV centres' absorption and emission are spin-dependent. We show how the varying absorption of the NV centres changes the Raman laser output. A shift in the diamond Raman laser threshold and output occurs with the external magnetic-field and microwave driving. We develop a theoretical framework including steady-state solutions to describe the effects of coheren…
This tutorial article provides a concise and pedagogical overview on negatively-charged nitrogen-vacancy (NV) centers in diamond. The research on the NV centers has attracted enormous attention for its application to quantum sensing, encompassing the areas of not only physics and applied physics but also chemistry, biology and life sciences. Nonetheless, its key technical aspects can be understood from the viewpoint of magnetic resonance. We focus on three facets of this ever-expanding research field, to which our viewpoint is especially relevant: microwave engineering, materials science, and …
Solid-state magnetometers like the Nitrogen-Vacancy center in diamond have been of paramount importance for the development of quantum sensing with nanoscale spatial resolution. The basic protocol is a Ramsey sequence, that imprints an external static magnetic field into phase of the quantum sensor, which is subsequently readout. In this work we show that the hyperfine coupling between the Nitrogen-Vacancy and a nearby Carbon-13 can be used to set a post-selection protocol that leads to an enhancement of the sensitivity under realistic experimental conditions. We found that for an isotopically…
Diamond nitrogen-vacancy (NV) center magnetometry has recently received considerable interest from researchers in the fields of applied physics and sensors. The purpose of this review is to analyze the principle, sensitivity, technical development potential, and application prospect of the diamond NV center magnetometry. This review briefly introduces the physical characteristics of NV centers, summarizes basic principles of the NV center magnetometer, analyzes the theoretical sensitivity, and discusses the impact of technical noise on the NV center magnetometer. Furthermore, the most critical…
Nitrogen-vacancy (NV) centers in millimeter-scale diamond samples were produced by irradiation and subsequent annealing under varied conditions. The optical and spin relaxation properties of these samples were characterized using confocal microscopy, visible and infrared absorption, and optically detected magnetic resonance. The sample with the highest NV- concentration, approximately 16 ppm = 2.8 x 10^{18} cm^{-3}, was prepared with no observable traces of neutrally-charged vacancy defects. The effective transverse spin relaxation time for this sample was T2* = 118(48) ns, predominately limit…
Microwave-free vector magnetometry and crystal orientation determination with Nitrogen-Vacancy centers using Bayesian inference
Universidad Carlos III de Madrid（马德里卡洛斯三世大学）；Helmholtz-Institute, GSI Helmholtzzentrum fur Schwerionenforschung（亥姆霍兹研究所，GSI重离子研究中心）；Johannes Gutenberg-Universität Mainz（美因茨约翰内斯古腾堡大学）；Department of Physics, University of California, Berkeley（加州大学伯克利分校物理系）
We present a protocol to achieve double quantum magnetometry at large static magnetic fields. This is a regime where sensitive sample parameters, such as the chemical shift, get enhanced facilitating their characterization. In particular, our method delivers two-tone stroboscopic radiation patterns with modulated Rabi frequencies to achieve larger spectral signals. Furthermore, it does not introduce inhomogeneous broadening in the sample spectrum preventing signal misinterpretation. Moreover, our protocol is designed to work under realistic conditions such as the presence of moderate microwave…
High-contrast absorption magnetometry in the visible to near-infrared range with nitrogen-vacancy ensembles
Fraunhofer Institute for Applied Solid State Physics IAF（弗劳恩霍夫应用固态物理研究所）；TECNALIA, Basque Research and Technology Alliance (BRTA)（巴斯克研究与技术联盟 TECNALIA）；College of Staten Island (CUNY)（史泰登岛学院（CUNY））；National Institutes for Quantum Science and Technology (QST)（量子科学技术研究开发机构）；Department of Materials Science, Tohoku University（东北大学材料科学系）
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 nitrogen-vacancy (NV) center in diamond allows room-temperature wide-field quantum magnetometry and metrology for a small volume, which is an important technology for applications in biology. Although coherence of the NV center has a limited frequency resolution of diamond magnetometry to 10-100 kHz, recent studies have shown that a phase sensitive protocol can beat the coherence limit on a confocal setup. Here, we report a new measurement protocol, "iQdyne," for improving the frequency resolution of wide-field imaging beyond the coherence limit of the NV center. We demonstrate wide-field …
New magnetometry techniques based on Nitrogen Vacancy (NV) defects in diamond have received much attention of late as a means to probe nanoscale magnetic environments. The sensitivity of a single NV magnetometer is primarily determined by the transverse spin relaxation time, $T_2$. Current approaches to improving the sensitivity employ crystals with a high NV density at the cost of spatial resolution, or extend $T_2$ via the manufacture of novel isotopically pure diamond crystals. We adopt a complementary approach, in which optimal dynamic decoupling techniques extend coherence times out to th…
Unconditional full vector magnetometry using spin selectivity in Nitrogen Vacancy centers in diamond
University of the Basque Country（巴斯克大学）；Centro de Fisica de Materiales (CFM), CSIC-UPV/EHU（材料物理中心，西班牙国家研究委员会/巴斯克大学）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；IKERBASQUE, Basque Foundation for Science（伊卡巴斯基克，巴斯克科学基金会）
Adaptive feedback normally provides the greatest accuracy for optical phase measurements. New advances in nitrogen vacancy centre technology have enabled magnetometry via individual spin measurements, which are similar to optical phase measurements but with low visibility. The adaptive measurements that previously worked well with high-visibility optical interferometry break down and give poor results for nitrogen vacancy centre measurements. We use advanced search techniques based on swarm optimisation to design better adaptive measurements that can provide improved measurement accuracy with …
The nitrogen vacancy (NV) center in diamond has emerged as a leading solid-state quantum sensor for applications including magnetometry, electrometry, thermometry, and chemical sensing. However, an outstanding challenge for practical applications is that existing NV-based sensing techniques require bulky and discrete instruments for spin control and detection. Here, we address this challenge by integrating NV based quantum sensing with complementary metal-oxide-semiconductor (CMOS) technology. Through tailored CMOS-integrated microwave generation and photodetection, this work dramatically redu…
We present a new magnetometry method integrating an ensemble of nitrogen-vacancy (NV) centers in a single-crystal diamond with an extended dynamic range for monitoring the fast changing magnetic-field. The NV-center spin resonance frequency is tracked using a closed-loop frequency locked technique with fast frequency hopping to achieve a 10 kHz measurement bandwidth, thus, allowing for the detection of fast changing magnetic signals up to 0.723 T/s.This technique exhibits an extended dynamic range subjected to the working bandwidth of the microwave source. This extended dynamic range can reach…
Continuous-wave AC magnetometry up to hundreds of megahertz using nitrogen-vacancy centers under a strong transverse magnetic field
School of Fundamental Science and Technology, Keio University（庆应义塾大学基础科学与技术学院）；Center for Spintronics Research Network, Keio University（庆应义塾大学自旋电子学研究网络中心）；Department of Electrical, Electronic, and Communication Engineering, Faculty of Advanced Science and Engineering, Chuo University（中央大学理工学部电气·电子·通信工程系）；Advanced Research Center for Diamond Science and Technology, Kanazawa University（金泽大学金刚石科学技术高级研究中心）
