Nitrogen-vacancy Centers Research Articles

Wide-field Fourier magnetic imaging with electron spins in diamond

Wide-field magnetic imaging based on nitrogen-vacancy (NV) centers in diamond has been shown the applicability in material and biological science. However, the spatial resolution is limited by the optical diffraction limit (>200 nm) due to the optical real-space localization and readout of NV centers. Here, we report the wide-field Fourier magnetic imaging technique to improve spatial resolution beyond the optical diffraction limit while maintaining the large field of view. Our method relies on wide-field pulsed magnetic field gradient encoding of NV spins and Fourier transform under pixel-dependent spatial filters. We have improved spatial resolution by a factor of 20 compared to the optical resolution and demonstrated the wide-field super-resolution magnetic imaging of a gradient magnetic field. This technique paves a way for efficient magnetic imaging of large-scale fine structures at the nanoscale.

Super-Resolution Diamond Magnetic Microscopy of Superparamagnetic Nanoparticles.

Scanning-probe and wide-field magnetic microscopes based on nitrogen-vacancy (NV) centers in diamond have enabled advances in the study of biology and materials, but each method has drawbacks. Here, we implement an alternative method for nanoscale magnetic microscopy based on optical control of the charge state of NV centers in a dense layer near the diamond surface. By combining a donut-beam super-resolution technique with optically detected magnetic resonance spectroscopy, we imaged the magnetic fields produced by single 30 nm iron-oxide nanoparticles. The magnetic microscope has a lateral spatial resolution of ∼100 nm, and it resolves the individual magnetic dipole features from clusters of nanoparticles with interparticle spacings down to ∼190 nm. The magnetic feature amplitudes are more than an order of magnitude larger than those obtained by confocal magnetic microscopy due to the narrower optical point-spread function and the shallow depth of NV centers. We analyze the magnetic nanoparticle images and sensitivity as a function of the microscope's spatial resolution and show that the signal-to-noise ratio for nanoparticle detection does not degrade as the spatial resolution improves. We identify sources of background fluorescence that limit the present performance, including diamond second-order Raman emission and imperfect NV charge state control. Our method, which uses <10 mW laser power and can be parallelized by patterned illumination, introduces a promising format for nanoscale magnetic imaging.

Synthesis and nitrogen content regulation of diamond in a high-pressure hydrogen-rich environment

The regulating nitrogen content of diamond in a hydrogen-rich high-temperature and high-pressure (HPHT) growth environment was systematically investigated in this work by developing three growth systems, namely, “FeNi+Ti”, “FeNi+C3N6H6”, and “FeNi+Ti+C3N6H6”. Optical microscopy, infrared spectroscopy, and photoluminescence (PL) spectroscopy measurements were conducted to analyze the spectroscopic characteristics of diamonds grown in these three systems. From our analysis, it was demonstrated that the presence of hydrogen in the sp3 hybrid C–H does not directly affect the color of the diamond and facilitates the increase of the nitrogen-vacancy (NV) center concentration in a high-nitrogen-content diamond. In addition, titanium plays an important role in nitrogen removal, while its impact on hydrogen doping within the diamond lattice is insignificant. Most importantly, by regulating the ratio of nitrogen impurities that coexist in the nitrogen and hydrogen HPHT environment, the production of hydrogenous IIa-type diamond, hydrogenous Ib-type diamond, and hydrogenous high-nitrogen-type diamonds was achieved with a nitrogen content of less than 1 ppm to 1600 ppm.

Triple electromagnetically induced transparency generated slow light for multiple carbon nanotube resonators

Hybrid spin-mechanical systems offer a promising platform for advancing quantum science and technology. However, practical implementation of applications within these hybrid quantum systems demands the seamless integration of supplementary physical components. In this context, we present a proposal for a multi-mode spin-mechanical setup, featuring the utilization of three-mode coupling nanomechanical carbon nanotube (CNT) resonators. These resonators interact with each other via a phase-dependent phonon-exchange mechanism, which is coupled to the same nitrogen vacancy (NV) centers in diamond. Based on the modulation of the phonon–phonon coupling phase and leveraging the triple Fano-like resonance phenomenon, a tripling of electromagnetically induced transparency (EIT) becomes achievable within the system. This tripling is accompanied by swift dispersion, leading to a subtle advancement or delay in outcomes. The phenomenon of triple Fano-like resonance, alongside the resulting triple EIT, engenders noteworthy slow-to-fast and fast-to-slow light effects, which is theoretically demonstrated in CNT resonators, with both identical and distinct frequencies. The findings underscore that CNT resonators with varying frequencies can evoke a more pronounced transition in the slow–fast–slow and fast–slow–fast light effects. This study lays the foundation for the application of phonon-mediated optical information storage and processing.

Stability of Near-Surface Nitrogen Vacancy Centers Using Dielectric Surface Passivation.

We study the photophysical stability of ensemble near-surface nitrogen vacancy (NV) centers in diamond under vacuum and air. The optically detected magnetic resonance contrast of the NV centers was measured following exposure to laser illumination, showing opposing trends in air compared to vacuum (increasing by up to 9% and dropping by up to 25%, respectively). Characterization using X-ray photoelectron spectroscopy (XPS) suggests a surface reconstruction: In air, atmospheric oxygen adsorption on a surface leads to an increase in NV- fraction, whereas in vacuum, net oxygen desorption increases the NV0 fraction. NV charge state switching is confirmed by photoluminescence spectroscopy. Deposition of ∼2 nm alumina (Al2O3) over the diamond surface was shown to stabilize the NV charge state under illumination in either environment, attributed to a more stable surface electronegativity. The use of an alumina coating on diamond is therefore a promising approach to improve the resilience of NV sensors.

Scattering of Ultrashort X-ray Pulses from Oriented NV Centers in the Diamond Structure

It is well known that the basis of diffraction analysis of matter is scattering, including the scattering of ultrashort laser pulses. In the theory of scattering of ultrashort pulses, the pulse duration parameter is usually not taken into account, which leads to some error. This error may be more significant than the considered effects in the scattering of the pulse on the studied structure. In this paper, it is shown that the pulse duration parameter should be taken into account when scattering X-ray pulses on oriented diamonds with NV centers. It is shown that the scattering spectra can be used to judge the orientation of NV centers in the diamond structure. The obtained results may be very different from the widely used theory of diffraction analysis, which confirms the necessity of taking into account the pulse duration parameter in the diagnosis of complex structures.

Indirect interaction of 13C nuclear spins in diamond with NV centers: simulation of the full J-coupling tensors

Recent experiments on the detection, imaging, characterization and control of multiple 13C nuclear spins, as well as of individual 13C–13C dimers in diamond using a single nitrogen-vacancy (NV) center as a sensor, along with the impressive progress in increasing the spectral resolution of such sensor (up to sub-Hertz), have created a request for detailed knowledge of all possible spin interactions in the studied systems. Here, we focus on the indirect interaction (J-coupling) of 13C nuclear spins in diamond, which was not previously taken into account in studies of NV centers. Using two different levels of the density functional theory (DFT), we simulated the full tensors nJKL (K, L = X, Y,Z), describing n-bond J-coupling of nuclear spins 13C in H-terminated diamond-like clusters C10H16 (adamantane) and C35H36, as well as in the cluster C33[NV−]H36 hosting the negatively charged NV− center. We found that, in addition to the usually considered isotropic scalar nJ-coupling constant, the anisotropic contributions to the nJ-coupling tensor are essential. We also showed that the presence of the NV center affects the J-coupling characteristics, especially in the case of 13C–13C pairs located near the vacancy of the NV center.

Single-Shot Readout of a Solid-State Electron Spin Qutrit.

Quantum systems usually feature a rich multilevel structure with promising resources for developing superior quantum technologies compared with their binary counterpart. Single-shot readout of these high-dimensional quantum systems is essential for exploiting their potential. Although there have been various high-spin systems, the single-shot readout of the overall state of high-spin systems remains a challenging issue. Here we demonstrate a reliable single-shot readout of spin qutrit state in a low-temperature solid-state system utilizing a binary readout scheme. We achieve a single-shot readout of an electron spin qutrit associated with a single nitrogen-vacancy center in diamond with an average fidelity of 87.80%. We use this spin qutrit system to verify quantum contextuality, a fundamental test of quantum mechanics. We observe a violation of the noncontextual hidden variable inequality with the developed single-shot readout in contrast to the conventional binary readout. These results pave the way for developing quantum information processing based on spin qutrits.

Control of an Environmental Spin Defect beyond the Coherence Limit of a Central Spin

Electronic spin defects in the environment of an optically active spin can be used to increase the size and hence the performance of solid-state quantum registers, especially for applications in quantum metrology and quantum communication. Previous works on multiqubit electronic spin registers in the environment of a nitrogen-vacancy (NV) center in diamond have only included spins directly coupled to the NV. As this direct coupling is limited by the central spin coherence time, it significantly restricts the maximum attainable size of the register. To address this problem, we present a scalable approach to increase the size of electronic spin registers. Our approach exploits a weakly coupled probe spin together with double-resonance control sequences to mediate the transfer of spin polarization between the central NV spin and an environmental spin that is not directly coupled to it. We experimentally realize this approach to demonstrate the detection and coherent control of an unknown electronic spin outside the coherence limit of a central NV. Our work paves the way for engineering larger quantum spin registers with the potential to advance nanoscale sensing, enable correlated noise spectroscopy for error correction, and facilitate the realization of spin-chain quantum wires for quantum communication. Published by the American Physical Society 2024

On the coupling between magnetoelastic waves and nitrogen vacancy centers in diamond

We show that a coupling exists between nitrogen vacancy (NV) centers in diamond in proximity to magnetoelastic spin waves generated by a voltage driven surface acoustic wave. Experimental measurements show the presence of coupling driven by both dipolar fields induced by a spin wave-like excitation and off-resonant coupling of the NV energy levels driven by acoustically driven ferromagnetic resonance dynamics. A model is proposed based on chiral coupling of the NV centers to the stray field that originates from a propagating magnetoelastic wave in a thin magnet, and model predictions are validated by experimental observations. Understanding of the coupling enables a direct measurement of the stray field polarization, which in turn provides a detailed picture of the resonantly coupled magnon–phonon interaction.

Research on optical fiber current transducer using nv center in diamond

Diamond nitrogen-vacancy (NV) center has been widely employed in experimental magnetic field measurement using continuous wave optical detection magnetic resonance (ODMR), which makes it possible for current sensing. An optical fiber current transducer prototype using an NV center is built for electric power application. The DC measurement with an error of less than 4% within 500 A is realized, in which the error of 50 A to 450 A is better than 2%, and the low-frequency AC measurement is preliminarily realized. In this essay, the accuracy of low current measurement is primarily affected by system noise, while the accuracy of heavy current is mainly affected by the width of the ODMR resonance peak. Optimizing the optical path as well as sensing structure meanwhile updating the demodulation algorithm of the measured data is the following work to improve the measurement accuracy.

Modelling Rabi oscillations for widefield radiofrequency imaging in nitrogen-vacancy centers in diamond

In this paper we study the dynamics of an ensemble of nitrogen-vacancy centers in diamond when its photoluminescence is detected by means of a widefield imaging system. We develop a seven-level model and use it to simulate the widefield detection of nitrogen-vacancy centers Rabi oscillations. The simulation results are compared with experimental measurements showing a good agreement. In particular, we use the model to explain the asymmetric shape of the detected Rabi oscillations due to an incomplete repolarization of the nitrogen-vacancy center during the pulse sequence implemented for the detection of Rabi oscillations.

Field-programmable-gate-array based hardware platform for nitrogen-vacancy center based fast magnetic imaging

A nitrogen-vacancy center based scanning magnetic microscope can be used to characterize magnetics at the nanoscale with high sensitivity. This paper reports a field-programmable-gate-array based hardware system that is designed to realize control and signal readout for fast scanning magnetic imaging with a nitrogen-vacancy center. A 10-channel 1 Msps @ 20 bit analog signal generator, a 12-channel 50 ps resolution pulse generator, a 300 Msps @ 16 bit lock-in amplifier with proportional integral derivative control function, and a 4-channel 200 Msps counter are integrated on the platform. A customized acceleration algorithm is realized with the re-configurable field-programmable-gate-array chip to accelerate the imaging speed of the nitrogen-vacancy system, and the experimental results prove that the imaging efficiency can be accelerated by five times compared to the system without the acceleration algorithm. The platform has considerable potential for future applications of fast scanning magnetic imaging.

Enhancing polarization transfer from nitrogen-vacancy centers to external nuclear spins via dangling bond mediators

The use of nitrogen-vacancy (NV) centers in diamond as a non-invasive platform for hyperpolarizing nuclear spins in molecular samples is a promising area of research with the potential to enhance the sensitivity of nuclear magnetic resonance (NMR) experiments. Transferring NV polarization out of the diamond structure has been achieved on nanoscale targets using dynamical nuclear polarization methods, but extending this polarization transfer to relevant NMR volumes poses significant challenges. One major technical hurdle is the presence of paramagnetic defects in the diamond surface which interfere with polarization outflow. However, these defects can be harnessed as intermediaries for the interaction between NVs and nuclear spins. We present a method that benefits from existing microwave sequences, namely the PulsePol, to transfer polarization efficiently and robustly using dangling bonds or other localized electronic spins, with the potential to increase polarization rates under realistic conditions.

Quantum-enhanced diamond molecular tension microscopy for quantifying cellular forces.

The constant interplay and information exchange between cells and the microenvironment are essential to their survival and ability to execute biological functions. To date, a few leading technologies such as traction force microscopy, optical/magnetic tweezers, and molecular tension-based fluorescence microscopy are broadly used in measuring cellular forces. However, the considerable limitations, regarding the sensitivity and ambiguities in data interpretation, are hindering our thorough understanding of mechanobiology. Here, we propose an innovative approach, namely, quantum-enhanced diamond molecular tension microscopy (QDMTM), to precisely quantify the integrin-based cell adhesive forces. Specifically, we construct a force-sensing platform by conjugating the magnetic nanotags labeled, force-responsive polymer to the surface of a diamond membrane containing nitrogen-vacancy centers. Notably, the cellular forces will be converted into detectable magnetic variations in QDMTM. After careful validation, we achieved the quantitative cellular force mapping by correlating measurement with the established theoretical model. We anticipate our method can be routinely used in studies like cell-cell or cell-material interactions and mechanotransduction.

Three-dimensional magnetic resonance tomography with sub-10 nanometer resolution

We demonstrate three-dimensional magnetic resonance tomography with a resolution down to 5.9 ± 0.1 nm. Our measurements use lithographically fabricated microwires as a source of three-dimensional magnetic field gradients, which we use to image NV centers in a densely doped diamond by Fourier-accelerated magnetic resonance tomography. We also demonstrate a compressed sensing scheme, which allows for direct visual interpretation without numerical optimization and implements an effective zoom into a spatially localized volume of interest, such as a localized cluster of NV centers. It is based on aliasing induced by equidistant undersampling of k-space. The resolution achieved in our work is comparable to the best existing schemes of super-resolution microscopy and approaches the positioning accuracy of site-directed spin labeling, paving the way to three-dimensional structure analysis by magnetic-gradient based tomography.

Compact and Fully Integrated LED Quantum Sensor Based on NV Centers in Diamond

Quantum magnetometry based on optically detected magnetic resonance (ODMR) of nitrogen vacancy centers in diamond nano or microcrystals is a promising technology for sensitive, integrated magnetic-field sensors. Currently, this technology is still cost-intensive and mainly found in research. Here we propose one of the smallest fully integrated quantum sensors to date based on nitrogen vacancy (NV) centers in diamond microcrystals. It is an extremely cost-effective device that integrates a pump light source, photodiode, microwave antenna, filtering and fluorescence detection. Thus, the sensor offers an all-electric interface without the need to adjust or connect optical components. A sensitivity of 28.32nT/Hz and a theoretical shot noise limited sensitivity of 2.87 nT/Hz is reached. Since only generally available parts were used, the sensor can be easily produced in a small series. The form factor of (6.9 × 3.9 × 15.9) mm3 combined with the integration level is the smallest fully integrated NV-based sensor proposed so far. With a power consumption of around 0.1W, this sensor becomes interesting for a wide range of stationary and handheld systems. This development paves the way for the wide usage of quantum magnetometers in non-laboratory environments and technical applications.

Fabrication of high-density nitrogen-vacancy (NV) center-enriched diamond particles through methyl trityl amine (C20H19N) seeding

Diamond particles (DPs) show promise for advanced applications in bioimaging and quantum sensing due to the presence of defect centers. This work reports a unique growth process for diamond particles composed of nitrogen-vacancy centers (NV-DPs) using a methyl trityl amine (C20H19N) diamondoid seed, which acts as a nitrogen source for NV creation. Growth was performed via microwave plasma-assisted chemical vapor deposition in a CH4/H2 plasma. Tantalum plates were chosen as the substrate to facilitate the release of the NV-rich DPs after growth. Raman spectra of NV-DPs grown at 550 °C showed a sharp, intense peak at ∼1334 cm−1, while those grown at 750 °C exhibited a broader, high intensity peak at 1336 cm−1. Photoluminescence revealed the formation of high-density NV centers, with the highest intensity for NV-DPs grown at 750 °C and 20 Torr. Optically detected magnetic resonance confirmed the presence of NV centers, especially for DPs grown at 750 °C. This seeding process enables precise nitrogen incorporation into diamond crystals to generate required spin properties by growing high-quality, well-faceted NV-DPs with customizable NV densities.

Frequency-tunable magnetic field sensing using continuous-wave optically detected magnetic resonance with nitrogen-vacancy centers in diamond

The nitrogen-vacancy (NV) center is a promising candidate to realize practical quantum sensors with high sensitivity and high spatial resolution at room temperature and atmospheric pressure. In conventional high-frequency AC magnetometry with NV centers, the setup requires a pulse sequence with an appropriate time synchronization and strong microwave power. To avoid these practical difficulties, AC magnetometry using continuous-wave optically detected magnetic resonance (CW-ODMR) was recently demonstrated. That previous study utilized radio frequency (RF)-dressed states generated by the coherent interaction between the electron spin of the NV center and the RF wave. However, the drawback of this method is that the detectable frequency of the AC magnetic fields is fixed. Here, we propose and demonstrate frequency-tunable magnetic field sensing based on CW-ODMR. In the new sensing scheme, we obtain RF double-dressed states by irradiation with RF fields at two different frequencies. One creates the RF-dressed states and changes the frequency of the target AC field. The other is a target AC field that induces a change in the CW-ODMR spectrum by generating the RF double-dressed states through coherent interaction with the RF-dressed states. The sensitivity of our method is estimated to be comparable to or even higher than that of the conventional method based on the RF field with a single frequency. The estimated bandwidth is 7.5 MHz, higher than that of the conventional method using the RF-dressed states. Our frequency-tunable magnetic field sensor based on CW-ODMR paves the way for new applications in diamond devices.

Creation of color centers in diamond by recoil implantation through dielectric films

The need of near-surface color centers in diamond for quantum technologies motivates the controlled doping of specific extrinsic impurities into the crystal lattice. Recent experiments have shown that this can be achieved by momentum transfer from a surface precursor via ion implantation, an approach known as “recoil implantation.” Here, we extend this technique to incorporate dielectric precursors for creating nitrogen-vacancy (NV) and silicon-vacancy (SiV) centers in diamond. Specifically, we demonstrate that gallium focused-ion-beam exposure to a thin layer of silicon nitride or silicon dioxide on the diamond surface results in the introduction of both extrinsic impurities and carbon vacancies. These defects subsequently give rise to near-surface NV and SiV centers with desirable properties after annealing.