Nitrogen-vacancy Spin Research Articles

Coherent Driving of a Single Nitrogen Vacancy Center by a Resonant Magnetic Tunnel Junction.

Nitrogen vacancy (NV) centers, atomic spin defects in diamond, represent an active contender for advancing transformative quantum information science (QIS) and innovations. One of the major challenges for designing NV-based hybrid systems for QIS applications results from the difficulty of realizing local control of individual NV spin qubits in a scalable and energy-efficient way. To address this bottleneck, we introduce magnetic tunnel junction (MTJ) devices to establish coherent driving of an NV center by a resonant MTJ with voltage controlled magnetic anisotropy. We show that the oscillating magnetic stray field produced by a resonant micromagnet can be utilized to effectively modify and drive NV spin rotations when the NV frequency matches the corresponding resonance conditions of the MTJ. Our results present a new pathway to achieve all-electric control of an NV spin qubit with reduced power consumption and improved solid-state scalability for implementing cutting-edge QIS technological applications.

Single and double quantum transitions in spin-mixed states under photo-excitation

Electronic spins associated with the Nitrogen-Vacancy (NV) center in diamond offer an opportunity to study spin-related phenomena with extremely high sensitivity owing to their high degree of optical polarization. Here, we study both single- and double-quantum transitions (SQT and DQT) in NV centers between spin-mixed states, which arise from magnetic fields that are non-collinear to the NV axis. We demonstrate the amplification of the ESR signal from both these types of transition under laser illumination. We obtain hyperfine-resolved X-band ESR signal as a function of both excitation laser power and misalignment of static magnetic field with the NV axis. This, combined with our analysis using a seven-level model that incorporates thermal polarization and double quantum relaxation, allows us to comprehensively analyze the polarization of NV spins under off-axis fields. Such detailed understanding of spin-mixed states in NV centers under photo-excitation can help greatly in realizing NV-diamond platform’s potential in sensing correlated magnets and biological samples, as well as other emerging applications, such as masing and nuclear hyperpolarization.

Quantum control and Berry phase of electron spins in rotating levitated diamonds in high vacuum

Levitated diamond particles in high vacuum with internal spin qubits have been proposed for exploring macroscopic quantum mechanics, quantum gravity, and precision measurements. The coupling between spins and particle rotation can be utilized to study quantum geometric phase, create gyroscopes and rotational matter-wave interferometers. However, previous efforts in levitated diamonds struggled with vacuum level or spin state readouts. To address these gaps, we fabricate an integrated surface ion trap with multiple stabilization electrodes. This facilitates on-chip levitation and, for the first time, optically detected magnetic resonance measurements of a nanodiamond levitated in high vacuum. The internal temperature of our levitated nanodiamond remains moderate at pressures below 10−5 Torr. We have driven a nanodiamond to rotate up to 20 MHz (1.2 × 109 rpm), surpassing typical nitrogen-vacancy (NV) center electron spin dephasing rates. Using these NV spins, we observe the effect of the Berry phase arising from particle rotation. In addition, we demonstrate quantum control of spins in a rotating nanodiamond. These results mark an important development in interfacing mechanical rotation with spin qubits, expanding our capacity to study quantum phenomena.

Plasmonically engineered nitrogen-vacancy spin readout.

Ultra-precise readout of single nitrogen-vacancy (NV) spins holds promise for major advancements in quantum sensing, computing, and communication technologies. Here we present a rigorous open quantum theory capable of simultaneously capturing the optical, vibronic, and spin interactions of the negatively charged NV center, both in the presence and absence of plasmonic interaction. Our theory is verified against existing experiments in the literature. We predict orders of magnitude brightness and contrast enhancements in optically detected magnetic resonance (ODMR) and NV spin qubit readout arising from plasmonic interaction. Such optimal enhancements occur in carefully engineered parameter regions, necessitating rigorous modelling prior to experimentation. Our theory equips the community with a tool to identify such regions.

Evolution of quantum spin sensing: From bench-scale ODMR to compact integrations

This paper provides a comprehensive review of quantum spin sensing with a focus on the nitrogen vacancy (NV) center in diamond. Beginning with the discovery of optically detected magnetic resonance in NV centers, we trace the evolution of this technology and its integration with complementary metal-oxide-semiconductor technology, marking a significant advancement in measurement science. The unique optical and spin properties of NV centers, operational at room temperature and under ambient conditions, have broadened their application spectrum, notably in magnetometry for nanoscale magnetic field detection. This work describes the transition from isolated NV centers to dense ensembles, highlighting the challenges and advancements in microfabrication and nanofabrication that have facilitated the integration of these centers with photonic structures and electronic devices. The efficient readout of NV spin states and the challenges in miniaturization are addressed, showcasing the development of compact, portable quantum sensors. We also discuss the potential impact of these sensors in various domains, including vehicle sensor systems and biomedical applications, underscoring the significance of environmental influences on magnetometric readings.

Detecting nitrogen-vacancy-hydrogen centers on the nanoscale using nitrogen-vacancy centers in diamond

In diamond, nitrogen defects like the substitutional nitrogen defect (Ns) or the nitrogen-vacancy-hydrogen complex (NVH) outnumber the nitrogen-vacancy (NV) defect by at least one order of magnitude creating a dense spin bath. While neutral Ns has an impact on the coherence of the NV spin state, the atomic structure of NVH reminds of a NV center decorated with a hydrogen atom. As a consequence, the formation of NVH centers could compete with that of NV centers possibly lowering the N-to-NV conversion efficiency in diamond grown with hydrogen-plasma-assisted chemical vapor deposition (CVD). Therefore, monitoring and controlling the spin bath is essential to produce and understand engineered diamond material with high NV concentrations for quantum applications. While the incorporation of Ns in diamond has been investigated on the nano- and mesoscale for years, studies concerning the influence of CVD parameters and the crystal orientation on the NVH formation have been restricted to bulk N-doped diamond providing high-enough spin numbers for electron paramagnetic resonance and optical absorption spectroscopy techniques. Here, we investigate submicron-thick (100)-diamond layers with nitrogen contents of (13.8±1.6)ppm and (16.7±3.6)ppm, and exploiting the NV centers in the layers as local nanosensors, we demonstrate the detection of NVH− centers using double electron-electron resonance (DEER). To determine the NVH− densities, we quantitatively fit the hyperfine structure of NVH− and confirm the results with the DEER method usually used for determining Ns0 densities. With our experiments, we access the spin bath composition on the nanoscale and enable a fast feedback loop in CVD recipe optimization with thin diamond layers instead of resource- and time-intensive bulk crystals. Furthermore, the quantification of NVH− plays a very important role for understanding the dynamics of vacancies and the incorporation of hydrogen into CVD diamond optimized for quantum technologies. Published by the American Physical Society 2024

Parallel pumping of magnons in inhomogeneous spin textures probed through NV spin relaxometry

We combine micromagnetic simulations and nitrogen-vacancy (NV) defect center spin relaxometry measurements to study magnon modes in inhomogeneous spin textures. A thin, micrometer-scale ferromagnetic disk is magnetized in a vortex state in which the magnetization curls around a central core. Micromagnetic simulations show that at zero applied field, the magnetization dynamics of the disk consist of a low frequency gyrotropic mode and higher frequency azimuthal magnon modes, all far detuned from the NV spin transition frequencies. An in-plane static magnetic field breaks the azimuthal symmetry of the vortex state, resulting in the magnon modes transforming in frequency and spatial profile as the field increases. Experimentally, we probe the dynamics of vortex magnetization as a function of applied in-plane static field and ac driving frequency by optically monitoring a nearby NV defect center spin. At certain values of the applied magnetic field, we observe enhanced spin relaxation when driving at twice the frequency of the NV ground state spin transition in optically detected magnetic resonance measurements. We attribute this effect to parallel pumping of a magnon mode in the disk producing magnons at half the excitation frequency. Micromagnetic simulations support this finding, showing spatial and spectral overlap of a confined magnon mode and an NV spin transition, with sufficient interaction strength to explain the observed signal.

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.

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

Third-order exceptional line in a nitrogen-vacancy spin system.

Exceptional points (EPs) are singularities in non-Hermitian systems, where k (k ≥ 2) eigenvalues and eigenstates coalesce. High-order EPs exhibit richer topological characteristics and better sensing performance than second-order EPs. Theory predicts even richer non-Hermitian topological phases for high-order EP geometries, such as lines or rings formed entirely by high-order EPs. However, experimental exploration of high-order EP geometries has hitherto proved difficult due to the demand for more degrees of freedom in the Hamiltonian's parameter space or a higher level of symmetries. Here we observe a third-order exceptional line in an atomic-scale system. To this end, we use a nitrogen-vacancy spin in diamond and introduce multiple symmetries in the non-Hermitian Hamiltonian realized with the system. Furthermore, we show that the symmetries play an essential role in the occurrence of high-order EP geometries. Our approach can in future be further applied to explore high-order EP-related topological physics at the atomic scale and, potentially, for applications of high-order EPs in quantum technologies.

Nanoscale Vector Magnetic Sensing with Current‐Driven Stochastic Nanomagnet

AbstractDetection of vector magnetic fields at nanoscale dimensions is critical in applications ranging from basic material science and fundamental physics to information storage and medical diagnostics. So far, nanoscale vector magnetic field sensing is achieved solely by exploiting a single nitrogen‐vacancy (NV) center in a diamond, by evaluating the Zeeman splitting of NV spin qubits by using the technique of an optically‐detected magnetic resonance. This protocol requires a complex optical setup and expensive detection systems to detect the photoluminescence light, which may limit miniaturization and scalability. Here, a simple approach with all‐electric operation to sensing a vector magnetic field at 200 × 200 nm2 dimensions is experimentally demonstrated, by monitoring a stochastic nanomagnet's transition probability from a metastable state, excited by a driving current due to spin‐orbit torque, to a settled state.

NV centres by vacancies trapping in irradiated diamond: experiments and modelling

Advances in applications of nitrogen-vacancy (NV) spin centres in diamond for sensing and quantum metrology depend critically on the NV fabrication methods. One such technique combines epitaxial diamond growth and electron or ion irradiation (He, C, etc), where NVs are activated by vacancy trapping at the nitrogen donor atoms upon thermal diffusion. In this work we study the efficiency of such method by analyzing NV depth profiles created by 340 keV and also 4 keV He irradiation in high purity CVD and HPHT diamond crystals and subjected to sequent annealing at 950 °C and 1200 °C temperatures. This analysis is coupled with the measurement of NV density in the bulk of CVD diamonds with nitrogen doping at low-ppb and low-ppm levels, exposed to MeV electrons in a wide range of the doses. For data analysis we developed an atomistic model based on probabilistic atomic jumps in a crystal lattice, which considers competitive trapping between di- (V2) or multi-vacancy defects compared to that of NVs. The efficiency of NV formation was defined as a ratio of the corresponding capture cross sections: σ NV vs. σV2 . Applying this model to the experimental data, the σNV/σV2 ratio was estimated about 0.1–0.5, where the activation energy of vacancy diffusion of about 1.7 eV was evaluated by 3D localization of individual NVs in depth profiles in a confocal microscope and sampling their spin coherence properties ( T2 ). In addition, we noted two subsidiary effects also discussed here: (i) reduction of NV density within the stopping range of the implanted He atoms after 1200∘ annealing and, (ii) partial suppression of NVs at near-surface areas visible only at low-dose electron exposures. The results of this study could be helpful to optimize the NV fabrication process reducing the density of ‘collateral’ lattice damage.

Mapping of Spin‐Wave Transport in Thulium Iron Garnet Thin Films Using Diamond Quantum Microscopy

AbstractSpin waves, collective dynamic magnetic excitations, offer crucial insights into magnetic material properties. Rare‐earth iron garnets offer an ideal spin‐wave (SW) platform with long propagation length, short wavelength, gigahertz frequency, and applicability to magnon spintronic platforms. Of particular interest, thulium iron garnet (TmIG) has attracted huge interest recently due to its successful growth down to a few nanometers, observed topological Hall effect, and spin‐orbit torque‐induced switching effects. However, there is no direct spatial measurement of its SW properties. This work uses diamond nitrogen‐vacancy (NV) magnetometry in combination with SW electrical transmission spectroscopy to study SW transport properties in TmIG thin films. NV magnetometry allows probing spin waves at the sub‐micrometer scale, seen by the amplification of the local microwave magnetic field due to the coupling of NV spin qubits with the stray magnetic field produced by the microwave‐excited spin waves. By monitoring the NV spin resonances, the SW properties in TmIG thin films are measured as a function of the applied magnetic field, including their amplitude, decay length (≈50 µm), and wavelength (0.8–2 µm). These results pave the way for studying spin qubit‐magnon interactions in rare‐earth magnetic insulators, relevant to quantum magnonics applications.

Local Control of a Single Nitrogen-Vacancy Center by Nanoscale Engineered Magnetic Domain Wall Motion.

Effective control and readout of qubits form the technical foundation of next-generation, transformative quantum information sciences and technologies. The nitrogen-vacancy (NV) center, an intrinsic three-level spin system, is naturally relevant in this context due to its excellent quantum coherence, high fidelity of operations, and remarkable functionality over a broad range of experimental conditions. It is an active contender for the development and implementation of cutting-edge quantum technologies. Here, we report magnetic domain wall motion driven local control and measurements of the NV spin properties. By engineering the local magnetic field environment of an NV center via nanoscale reconfigurable domain wall motion, we show that NV photoluminescence, spin level energies, and coherence time can be reliably controlled and correlated to the magneto-transport response of a magnetic device. Our results highlight the electrically tunable dipole interaction between NV centers and nanoscale magnetic structures, providing an attractive platform to realize interactive information transfer between spin qubits and nonvolatile magnetic memory in hybrid quantum spintronic systems.

Quantum diamond microscope for dynamic imaging of magnetic fields

Wide-field imaging of magnetic signals using ensembles of nitrogen-vacancy (NV) centers in diamond has garnered increasing interest due to its combination of micron-scale resolution, millimeter-scale field of view, and compatibility with diverse samples from across the physical and life sciences. Recently, wide-field NV magnetic imaging based on the Ramsey protocol has achieved uniform and enhanced sensitivity compared to conventional measurements. Here, we integrate the Ramsey-based protocol with spin-bath driving to extend the NV spin dephasing time and improve magnetic sensitivity. We also employ a high-speed camera to enable dynamic wide-field magnetic imaging. We benchmark the utility of this quantum diamond microscope (QDM) by imaging magnetic fields produced from a fabricated wire phantom. Over a 270 × 270 μm2 field of view, a median per-pixel magnetic sensitivity of 4.1(1) nT /Hz is realized with a spatial resolution ≲ 10 μm and sub-millisecond temporal resolution. Importantly, the spatial magnetic noise floor can be reduced to the picotesla scale by time-averaging and signal modulation, which enables imaging of a magnetic-field pattern with a peak-to-peak amplitude difference of about 300 pT. Finally, we discuss potential new applications of this dynamic QDM in studying biomineralization and electrically active cells.

Design and simulation of an accelerometer based on NV center spin–strain coupling

The nitrogen-vacancy (NV) center quantum systems have emerged as versatile tools in the field of precision measurement because of their high sensitivity in spin state detection and miniaturization potential as solid-state platforms. In this paper, an acceleration sensing scheme based on NV spin–strain coupling is proposed, which can effectively eliminate the influence of the stray noise field introduced by traditional mechanical schemes. Through the finite element simulation, it is found that the measurement bandwidth of this ensemble NV spin system ranges from 3 kHz to hundreds of kHz with structure optimization. The required power is at the sub-μW level, corresponding to a noise-limited sensitivity of 6.7×10−5g/Hz . Compared with other types of accelerometers, this micro-sized diamond sensor proposed here has low power consumption, exquisite sensitivity, and integration potential. This research opens a fresh perspective to realize an accelerometer with appealing comprehensive performance applied in biomechanics and inertial measurement fields.

Nitrogen-vacancy magnetometry of CrSBr by diamond membrane transfer

Magnetic imaging using nitrogen-vacancy (NV) spins in diamonds is a powerful technique for acquiring quantitative information about sub-micron scale magnetic order. A major challenge for its application in the research on two-dimensional (2D) magnets is the positioning of the NV centers at a well-defined, nanoscale distance to the target material required for detecting the small magnetic fields generated by magnetic monolayers. Here, we develop a diamond “dry-transfer” technique akin to the state-of-the-art 2D-materials assembly methods and use it to place a diamond micro-membrane in direct contact with the 2D interlayer antiferromagnet CrSBr. We harness the resulting NV-sample proximity to spatially resolve the magnetic stray fields generated by the CrSBr, present only where the CrSBr thickness changes by an odd number of layers. From the magnetic stray field of a single uncompensated ferromagnetic layer in the CrSBr, we extract a monolayer magnetization of MCSB = 0.46(2) T, without the need for exfoliation of monolayer crystals or applying large external magnetic fields. The ability to deterministically place NV-ensemble sensors into contact with target materials and detect ferromagnetic monolayer magnetizations paves the way for quantitative analysis of a wide range of 2D magnets assembled on arbitrary target substrates.

Frequency Limits of Sequential Readout for Sensing AC Magnetic Fields Using Nitrogen-Vacancy Centers in Diamond.

The nitrogen-vacancy (NV) centers in diamond have the ability to sense alternating-current (AC) magnetic fields with high spatial resolution. However, the frequency range of AC sensing protocols based on dynamical decoupling (DD) sequences has not been thoroughly explored experimentally. In this work, we aimed to determine the sensitivity of the ac magnetic field as a function of frequency using the sequential readout method. The upper limit at high frequency is clearly determined by Rabi frequency, in line with the expected effect of finite DD-pulse width. In contrast, the lower frequency limit is primarily governed by the duration of optical repolarization rather than the decoherence time (T2) of NV spins. This becomes particularly crucial when the repetition (dwell) time of the sequential readout is fixed to maintain the acquisition bandwidth. The equation we provide successfully describes the tendency in the frequency dependence. In addition, at the near-optimal frequency of 1 MHz, we reached a maximum sensitivity of 229 pT/Hz by employing the XY4-(4) DD sequence.

Improved Limits on an Exotic Spin- and Velocity-Dependent Interaction at the Micrometer Scale with an Ensemble-NV-Diamond Magnetometer.

Searching for exotic interactions provides a path for exploring new particles beyond the standard model. Here, we used an ensemble-NV-diamond magnetometer to search for an exotic spin- and velocity-dependent interaction between polarized electron spins and unpolarized nucleons at the micrometer scale. A thin layer of nitrogen-vacancy electronic spin ensemble in diamond is utilized as both the solid-state spin quantum sensor and the polarized electron source, and a vibrating lead sphere serves as the moving unpolarized nucleon source. The exotic interaction is searched by detecting the possible effective magnetic field induced by the moving unpolarized nucleon source using the ensemble-NV-diamond magnetometer. Our result establishes new bounds for the coupling parameter f_{⊥} within the force range from 5 to 400 μm. The upper limit of the coupling parameter at 100 μm is |f_{⊥}|≤1.1×10^{-11}, which is 3 orders of magnitude more stringent than the previous constraint. This result shows that NV ensemble can be a promising platform to search for hypothetical particles beyond the standard model.

Dressed-state control of effective dipolar interaction between strongly-coupled solid-state spins

Strong interactions between defect spins in many-body solid-state quantum systems are a crucial resource for exploring non-classical states. However, they face the key challenge of controlling interactions between the defect spins, since they are spatially fixed inside the host lattice. In this work, we present a dressed state approach to control the effective dipolar coupling between solid-state spins and demonstrate this scheme experimentally using two strongly-coupled nitrogen vacancy (NV) centers in diamond. Through Ramsey spectroscopy on the sensor spin, we detect the change of the effective dipolar field generated by the control spin prepared in different dressed states. To observe the change of interaction dynamics, we deploy spin-lock-based polarization transfer measurements between the two NV spins in different dressed states. This scheme allows us to control the distribution of interaction strengths in strongly interacting spin systems, which can be a valuable tool for generating multi-spin correlated states for quantum-enhanced sensing.