Ensemble Of Nitrogen-vacancy Centers Research Articles

Probing coherence properties of shallow implanted NV snsembles under different oxygen terminations

Abstract Nitrogen vacancy (NV) color centers in diamond have shown great potential for various applications in quantum technology due to their long coherence times, high sensitivity to magnetic fields and atomic scale resolution. However, one major challenge in utilizing near surface NV centers is the decoherence caused by spins and charges fluctuating on the surface, which affects the spin properties of the sensors. To reduce the induced noise, various oxygen surface treatments such as low power oxygen plasma treatment and annealing under oxygen atmosphere have been explored to terminate the diamond surface and reduce its impact on NV coherence. We showed that the NV center's coherence time can be enhanced up to a factor of 3 over a large spectral range of noise. Double electron electron resonance (DEER) measurements revealed an extra source of decoherence, scaling similarly as the P1 spin bath. The improvement in coherence times is accompanied with an increase in measured ketone/ether content and reduction of sp2 signal in X-ray photoelectron spectroscopy (XPS) measurements. Finally we compared the performance of different NV ensembles and surface treatments for sensing external proton spins. The oxygen annealing is an effective procedure of enhancing the spin coherence times and reducing broad band spin noise experienced by shallow implanted ensemble NV centers in diamond.

Utilizing the multifrequency resonances of the electron spins in diamond nitrogen-vacancy centers under strong radio frequency driving for quantum sensing

Multifrequency resonances in the pulsed-optically detected magnetic resonance (ODMR) spectra of electron spins in ensemble nitrogen-vacancy (NV) centers in diamonds are investigated under strong radio frequency (RF) driving at a MHz frequency range and weak microwave driving at a GHz frequency range in a bias static magnetic field for quantum sensing applications. First, we demonstrate that the coherent destruction of tunneling, which leads to the disappearance of the main resonance peaks, can be utilized for precise calibration of the RF amplitude. Next, we clarify the condition for enhancing the sensitivity of a DC magnetic field under strong RF driving at the RF frequency that matches the split frequency due to the hyperfine interaction between 15N nuclear spins and the NV electron spins. Our findings indicate that strong RF driving increases the sensitivity of the DC magnetic field by enhancing the ODMR contrast and reducing the linewidth. The above results contribute to certifying the quantitative accuracy of RF imaging and enhancing the sensitivity of the DC magnetic field imaging using ensemble NV centers in diamonds.

All-in-one quantum diamond microscope for sensor characterization

Ensembles of nitrogen-vacancy (NV) centers in diamond are a leading platform for sensing and imaging magnetic fields at room temperature, in part due to advances in diamond growth. An essential step to improving diamond material involves the characterization of crystal and NV-related properties, such as strain and paramagnetic impurities, which can shift and broaden the NV resonances used for sensing. Full sample characterization through wide-field imaging enables both fast and detailed feedback for growers, along with the estimation of sensing performance before use. We present a quantum diamond microscope tailored for millimeter-scale wide-field mapping of key quantum properties of NV-diamond chips, including NV ensemble photoluminescence intensity, spin-lattice relaxation time (T1), and spin-coherence lifetimes (T2 and T2*). Our design also allows for lattice stress/strain and birefringence magnitude/angle mapping, and their in situ correlation with NV properties.

Diamond Surfaces with Lateral Gradients for Systematic Optimization of Surface Chemistry for Relaxometry - a Low-Pressure Plasma-Based Approach.

Diamond is increasingly popular because of its unique material properties. Diamond defects called nitrogen vacancy (NV) centers allow for measurements with unprecedented sensitivity. However, to achieve ideal sensing performance, NV centers need to be within nanometers from the surface and are thus strongly dependent on the local surface chemistry. Several attempts have been made to compare diamond surfaces. However, due to the high price of diamond crystals with shallow NV centers, a limited number of chemical modifications have been studied. Here, we developed a systematic method to investigate the continuity of different local environments with varying densities and natures of surface groups in a single experiment on a single diamond plate. To achieve this goal, we used diamonds with a shallow ensemble of NV centers and introduced a chemical gradient across the surface. More specifically, we used air and hydrogen plasma. The gradients were formed by a low-pressure plasma treatment after masking with a right-angled triangular prism shield. As a result, the surface contained gradually more oxygen/hydrogen toward the open end of the shield. We then performed wide-field relaxometry to determine the effect of surface chemistry on the sensing performance. As expected, relaxation times and thus sensing performance indeed vary along the gradient.

J-coupling NMR spectroscopy with nitrogen vacancy centers at high fields

A diamond-based sensor utilizing nitrogen-vacancy (NV) center ensembles permits the analysis of micron-sized samples through nuclear magnetic resonance (NMR) techniques at room temperature. Current efforts are directed towards extending the operating range of NV centers into high magnetic fields, driven by the potential for larger nuclear spin polarization of the target sample and the presence of enhanced chemical shifts. Especially interesting is the access to J-couplings as they carry information of chemical connectivity inside molecules. In this work, we present a protocol to access J-couplings in both homonuclear and heteronuclear cases with NV centers at high magnetic fields. Our protocol leads to a clear spectrum exclusively containing J-coupling features with high resolution. This resolution is limited primarily by the decoherence of the target sample, which is mitigated by the noise-filtering capacities of our method. Published by the American Physical Society 2024

Gate-set evaluation metrics for closed-loop optimal control on nitrogen-vacancy center ensembles in diamond

A recurring challenge in quantum science and technology is the precise control of their underlying dynamics that lead to the desired quantum operations, often described by a set of quantum gates. These gates can be subject to application-specific errors, leading to a dependence of their controls on the chosen circuit, the quality measure and the gate-set itself. A natural solution would be to apply quantum optimal control in an application-oriented fashion. In turn, this requires the definition of a meaningful measure of the contextual gate-set performance. Therefore, we explore and compare the applicability of quantum process tomography, linear inversion gate-set tomography, randomized linear gate-set tomography, and randomized benchmarking as measures for closed-loop quantum optimal control experiments, using a macroscopic ensemble of nitrogen-vacancy centers in diamond as a test-bed. Our work demonstrates the relative trade-offs between those measures and how to significantly enhance the gate-set performance, leading to an improvement across all investigated methods.

Optimizing Control of a Hybrid Quantum System of Nitrogen-Vacancy Centers and Superconducting Transmon Qubits

Abstract The control of hybrid quantum systems via the application of external fields is rapidly evolving field of research for the development of quantum applications and technologies. We model and optimize the dynamics of a hybrid quantum system consists of two non-local ensembles of nitrogen-vacancy centers and a superconducting transmon qubit mediated by two transmission line resonators. We apply a set of optimized time-dependent external driving field to enhance the system performance to function as a high fidelity state-to-state transfer. The Hamiltonian of the externally driven transmission line resonators is modelled by considering the non-linear transmons. The numerical simulation of the system is done using the optimized parameters of the external fields. By applying the optimized pulses, we have increased the fidelity of the state transfer from 0.7 to 1.0 within 100 ns. By varying the full wave half maxima value (FWHM) of the Gaussian pulse, it result in decreasing the amplitude of the fast oscillating states of the transmon and nitrogen-vacancy ensembles. These optimized external pulses also created a strong coupling between the components of under-consideration physical quantum system, which will eventually increase the fidelity of the system in a relatively faster time.

Uniform microwave field formation for control of ensembles of negatively charged nitrogen vacancy in diamond.

The homogeneity of the microwave magnetic field is essential in controlling a large volume of ensemble spins, for example, in the case of sensitive magnetometry with nitrogen-vacancy (NV) centers in diamond. This is particularly important for pulsed measurement, where the fidelity of control pulses plays a crucial role in its sensitivity. So far, several magnetic field-forming systems have been proposed, but no detailed comparison has been made. Here, we numerically study the homogeneity of five different systems, including a planar antenna, a dielectric resonator, a cylindrical inductor, a barrel-shaped coil, and a nested barrel-shaped coil. The results of the simulation allowed us to optimize the design parameters of the barrel-shaped field-forming system, which led to significantly improved magnetic field uniformity. To measure this effect, we experimentally compared the homogeneity of a field-forming system having a barrel shape with that of a planar field-forming system by measuring Rabi oscillations of an ensemble of NV centers with them. Significant improvements in inhomogeneity were confirmed in the barrel-shaped coil.

Nitrogen-vacancy centers as a self-gauged micro-scale heater and its application for multi-modal sensing

The optical excitation of nitrogen-vacancy (NV) color centers in diamonds mostly results in fluorescence emission. During this process, a portion of the incident energy is transferred to phonon vibration, which heats the diamond crystal. For single NV color centers, the heat generated by the optical cycle is negligible, while for an ensemble of NV defects, the generated heat accumulates rapidly and heats the diamond. The temperature rise is rapid due to the high thermal conductivity of the diamond. In addition to the ability to be heated by light, the NV defect's unique properties also allow for the precise measurement of temperature using optically detected magnetic resonance. Here, we experimentally demonstrate that microcrystalline diamond containing NV center ensembles can be used as a self-gauged microheater. We attached a microcrystal diamond to an optical fiber in an endoscope configuration, evaluated its performance as a self-gauged heater under varied biologically relevant environments, and discussed its potential applications. In addition to the aforementioned capabilities, the NV defect enables the precise measurement of local magnetic fields. This provides a unique multimodal sensor to probe temperature-controlled magnetic phenomena at microscopic scales.

Making Use of Low‐Cost High‐Pressure–High‐Temperature‐Diamond Materials for Industry‐Type Quantum Sensor Device Applications

A cost‐effective approach to provide diamond platelets containing nitrogen vacancy center ensembles (NVs) in the range of ppm is investigated. Industry‐type high‐pressure–high‐temperature‐diamond type 1b containing a high number of interstitial nitrogen in the range of several tens of ppm are used and small diamond platelets (size ≈1 × 1 mm2, thickness ≈300 μm) are prepared by laser cutting and polishing. The nitrogen is converted into NV by means of high‐energy electron irradiation of 10 MeV and annealing at 900 °C. Variations in the irradiation dose between 0.5E18 1/cm2 and 2E18 1/cm2 result in different densities of NV. The diamond platelets are analyzed with regard to their nitrogen concentration and photoluminescence as well as optically detected magnetic resonance is used to investigate the usability for a NV‐based magnetometer. A method to calculate the ratio of negatively to neutrally charged NV (NV−/NV0) is proposed that uses the photoluminescence intensities of the spectrum at 575 and 638 nm, namely, the zero‐phonon lines of NV− and NV0.

Microscale fiber-integrated vector magnetometer with on-tip field biasing using N - V ensembles in diamond microcrystals

In quantum sensing of magnetic fields, ensembles of nitrogen-vacancy centers in diamond offer high sensitivity, high bandwidth and outstanding spatial resolution while operating in harsh environments. Moreover, the orientation of defect centers along four crystal axes forms an intrinsic coordinate system, enabling vector magnetometry within a single diamond crystal. While most vector magnetometers rely on a known bias magnetic field for full recovery of three-dimensional (3D) field information, employing external 3D Helmholtz coils or permanent magnets results in bulky, laboratory-bound setups, impeding miniaturization of the device. Here, a novel approach is presented that utilizes a fiber-integrated microscale coil at the fiber tip to generate a localized uniaxial magnetic field. The same fiber-tip coil is used in parallel for spin control by combining dc and microwave signals in a bias tee. To implement vector magnetometry using a uniaxial bias field, the orientation of the diamond crystal is preselected and then fully characterized by rotating a static magnetic field in three planes of rotation. The measurement of vector magnetic fields in the full solid angle is demonstrated with a shot-noise-limited sensitivity of 19.4nT/Hz1/2 and microscale spatial resolution while achieving a fiber sensor head cross section of less than 1mm2. Published by the American Physical Society 2024

Robust Hamiltonian Engineering for Interacting Qudit Systems

Dynamical decoupling and Hamiltonian engineering are well-established techniques that have been used to control qubit systems. However, designing the corresponding methods for qudit systems has been challenging due to the lack of a Bloch sphere representation, more complex interactions, and additional control constraints. By identifying several general structures associated with such problems, we develop a formalism for the robust dynamical decoupling and Hamiltonian engineering of strongly interacting qudit systems. Our formalism significantly simplifies qudit pulse-sequence design while naturally incorporating robustness conditions necessary for experimental practicality. We experimentally demonstrate these techniques in a strongly interacting, disordered ensemble of spin-1 nitrogen-vacancy centers, achieving more than an order-of-magnitude improvement in coherence time over existing pulse sequences. We further describe how our techniques enable the engineering of exotic many-body phenomena such as quantum many-body scars, and open up new opportunities for quantum metrology with enhanced sensitivities. These results enable wide-reaching new applications for dynamical decoupling and Hamiltonian engineering in many-body physics and quantum metrology. Published by the American Physical Society 2024

High dynamic-range and portable magnetometer using ensemble nitrogen-vacancy centers in diamond.

Nitrogen vacancy (NV) centers in diamonds have been explored for a wide range of sensing applications in the last decade due to their unique quantum properties. In this work, we report a compact and portable magnetometer with an ensemble of NV centers, which we call the Quantum MagPI (Quantum Magnetometer with Proportional Integral control). Our fully integrated compact sensor assembly and control electronics fit inside a 10 × 10 × 7cm3 box and a 30 × 25 × 5cm3 rack-mountable box, respectively. We achieve a bandwidth normalized sensitivity of ∼10 nT/Hz. Using closed-loop feedback for locking to the resonance frequency, we extend the linear dynamic range to 200 μT (20× improvement compared to the intrinsic dynamic range) without compromising the sensitivity. We report a detailed performance analysis of the magnetometer through measurements of noise spectra, Allan deviation, and tracking of nT-level magnetic fields in real-time. In addition, we demonstrate the utility of such a magnetometer by real-time tracking of the movement of an elevator car and door opening events by measuring the projection of the magnetic field along one of the NV-axes under ambient temperature and humidity conditions.

Near zero-field microwave-free magnetometry with ensembles of nitrogen-vacancy centers in diamond

Near zero-field microwave-free magnetometry with ensembles of nitrogen-vacancy centers in diamond

Microwave power self-coherent reference measurement based on ensembles of nitrogen-vacancy centers in diamond.

Microwave detection based on optical detection magnetic resonance technology (ODMR) of nitrogen-vacancy (NV) centers is simple and non-invasive. However, in high microwave power ranges, saturation appears and cannot be used for accurate power measurement. The self-coherent reference measurement for high-power microwave based on ODMR of NV centers has been demonstrated. Firstly, by introducing the principle of microwave self-coherent reference, that is, by adjusting the phase difference to achieve power regulation of microwave, a conversion model by phase modulation between enhancement and attenuation of microwave power is introduced. Then, the microwave self-coherent reference measurement is established under combinations of microwave power with different phase settings. Combined with the frequency modulation technology, the sensitivity of measurement is significantly improved from 4.59 nT/Hz1/2 to 67.69 pT/Hz1/2. The maximum measurement range of microwave power can be extended to 2×104 times the initial saturated power of direct measurement with ODMR. The results show that the method efficiently overcomes saturation under the direct measurement of ODMR and provides useful technical assistance for near-field detection, performance monitoring, and problem diagnostics for microwave devices.

Deep polarization of the ensemble nitrogen-vacancy centers in diamonds induced by an Airy beam with a long focal depth

Solid-state spin systems with nitrogen-vacancy (NV) centers in diamonds constitute an increasingly popular platform for quantum sensing. However, most existing platforms designed with ensemble NV centers exhibit a sensitivity that is significantly less than the theoretical maximum. This low sensitivity limits the expansion of the experimental results and application areas. In this study, the sensitivity is improved by increasing the pumping depth of the excitation beam to increase the number of particles involved in spin polarization at a given laser intensity. Compared with the proposed Airy beam with a long focal depth (25.46 λ) and the widely utilized Gauss beam pumping ensemble NV centers, the spin resonance factor fSR can be improved by 10.02%. This sensitivity-optimized approach enhances the functionality of sensors with NV centers.

Investigation of zero-phonon line characteristics in ensemble nitrogen-vacancy centers at 1.6 K–300 K

The ensemble of nitrogen-vacancy (NV) centers is widely used in quantum information transmission, high-precision magnetic field, and temperature sensing due to their advantages of long-lived state and the ability to be pumped by optical cycling. In this study, we investigate the zero-phonon line behavior of the two charge states of NV centers by measuring the photoluminescence of the NV center at 1.6 K-300 K. The results demonstrate a positional redshift, an increase in line width, and a decrease in fluorescence intensity for the ZPL of NV0 and NV- as the temperature increased. In the range of 10 K to 140 K, the peak shift with high concentrations of NV- revealed an anomaly of bandgap reforming. The peak position undergoes a blueshift and then a redshift as temperature increases. Furthermore, the transformation between NV0 and NV- with temperature changes has been obtained in diamonds with different nitrogen concentrations. This study explored the ZPL characteristics of NV centers in various temperatures, and the findings are significant for the development of high-resolution temperature sensing and high-precision magnetic field sensing in ensemble NV centers.

Searching for exotic spin-dependent interactions with diamond-based vector magnetometer

We propose a new method to search for exotic spin-spin interactions between electrons and nucleons using a diamond-based vector magnetometer. The vector magnetometer can be constructed from ensembles of nitrogen-vacancy centers along different axes in a diamond. The N14 nuclear spins of nitrogen-vacancy centers in the same diamond can be polarized through the dynamic nuclear polarization method to serve as spin sources. With the vector magnetometer, the sought-after exotic interactions can be distinguished from the magnetic dipole-dipole interaction. For the axion-mediated interaction VPP, new upper bounds of the coupling |gPegPN| are expected within the force range from 10 nm to 100 μm. For the Z′-mediated interaction VAA, new upper bounds of the coupling |gAegAN| are expected within the force range from 10 nm to 1 cm. The new upper bounds for VPP and VAA are both expected to be more than 5 orders of magnitude more stringent than existing constraints at the force range of 1 μm with the total measurement time of 1 day. Published by the American Physical Society 2024

Diamond surface functionalization via visible light–driven C–H activation for nanoscale quantum sensing

Nitrogen-vacancy (NV) centers in diamond are a promising platform for nanoscale NMR sensing. Despite significant progress toward using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. Such sensing requires that target molecules are immobilized within nanometers of NV centers with long spin coherence. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C-H bonds on single-crystal diamond surfaces under ambient conditions using visible light, forming C-F, C-Cl, C-S, and C-N bonds at the surface. This method is compatible with NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof-of-principle demonstration, we use shallow ensembles of NV centers to detect nuclear spins from surface-bound functional groups. Our approach to surface functionalization opens the door to deploying NV centers as a tool for chemical sensing and single-molecule spectroscopy.

Integrated coplanar waveguide coil on diamond for enhanced homogeneous broadband NV magnetometry.

Nitrogen-vacancy (NV) centers in diamond have emerged as promising quantum sensors due to their highly coherent and optically addressable spin states with potential applications in high-sensitivity magnetometry. Homogeneously addressing large ensembles of NV centers offers clear benefit in terms of sensing precision as well as in fundamental studies of collective effects. Such experiments require a spatially uniform, intense, and broadband microwave field that can be difficult to generate. Previous approaches, such as copper wires, loop coils, and planar structures, have shown limitations in field homogeneity, bandwidth, and integration in compact devices. In this paper, we present a coplanar waveguide (CPW) gold coil patterned on a 3 × 3 mm 2 diamond substrate, offering full integration, enhanced stability, and broad bandwidth suitable for various NV sensing applications. Coil fabricated on diamond offers several advantages for magnetometry with NV centers ensemble, including enhanced heat dissipation, seamless integration, scalability, and miniaturization potential. We optimize critical geometrical parameters to achieve a homogeneous magnetic field with a coefficient of variation of less than 6% over an area of 0.5 mm 2 and present experimental results confirming the performance of the proposed CPW coil.