Single Nitrogen-vacancy Center Research Articles

Quantum estimation of tripartite coupling in spin-magnon-mechanical hybrid systems

Tripartite interactions play a fundamental role in the quantum information processing and quantum technology. However, it is generally difficult to realize strong tripartite coupling. We investigate the estimation of a tripartite coupling strength in a hybrid setup composed of a single nitrogen-vacancy (NV) center and a micromagnet. A time-independent parametric drive can be utilized to increase the estimation precision of the tripartite coupling strength. By calculating the quantum Fisher information (QFI), we can obtain the optimal estimation precision by measuring the eigenstate of the tripartite system. At the critical position, the QFI is divergent due to that the preparation time of the eigenstate is divergent. When the system is subjected to a dissipation, the QFI near the critical point of the driven-dissipation phase transition is analytically obtained. The direct intensity measurement is the optimal measurement near the dissipation phase transition point. In addition, we quantify the robustness of an imperfect measurement operator by the measurement noise susceptibility based on the error propagation formula. We find that the direct intensity measurement is robust enough against small measurement disturbance from a coherent drive. But it can be disturbed by the nonlinear anti-harmonic measurement noise, especially near the critical point.

Sensing at the Nanoscale Using Nitrogen-Vacancy Centers in Diamond: A Model for a Quantum Pressure Sensor.

The sensing of stress under harsh environmental conditions with high resolution has critical importance for a range of applications including earth's subsurface scanning, geological CO2 storage monitoring, and mineral and resource recovery. Using a first-principles density functional theory (DFT) approach combined with the theoretical modelling of the low-energy Hamiltonian, here, we investigate a novel approach to detect unprecedented levels of pressure by taking advantage of the solid-state electronic spin of nitrogen-vacancy (NV) centers in diamond. We computationally explore the effect of strain on the defect band edges and band gaps by varying the lattice parameters of a diamond supercell hosting a single NV center. A low-energy Hamiltonian is developed that includes the effect of stress on the energy level of a ±1 spin manifold at the ground state. By quantifying the energy level shift and split, we predict pressure sensing of up to 0.3 MPa/Hz using the experimentally measured spin dephasing time. We show the superiority of the quantum sensing approach over traditional optical sensing techniques by discussing our results from DFT and theoretical modelling for the frequency shift per unit pressure. Importantly, we propose a quantum manometer that could be useful to measure earth's subsurface vibrations as well as for pressure detection and monitoring in high-temperature superconductivity studies and in material sciences. Our results open avenues for the development of a sensing technology with high sensitivity and resolution under extreme pressure limits that potentially has a wider applicability than the existing pressure sensing technologies.

Digital noise spectroscopy with a quantum sensor

We introduce and experimentally demonstrate a quantum sensing protocol to sample and reconstruct the autocorrelation of a noise process using a single-qubit sensor under digital control modulation. This Walsh noise spectroscopy method exploits simple sequences of spin-flip pulses to generate a complete basis of digital filters that directly sample the power spectrum of the target noise in the sequency domain, from which the autocorrelation function in the time domain, as well as the power spectrum in the frequency domain, can be reconstructed using linear transformations. Our method, which can also be seen as an implementation of frame-based noise spectroscopy, solves the fundamental difficulty in sampling continuous functions with digital filters by introducing a transformation that relates the arithmetic and logical time domains. In comparison to standard, frequency-based dynamical-decoupling noise spectroscopy protocols, the accuracy of our method is only limited by sampling and discretization in the time domain and can be easily improved, even under limited evolution time due to decoherence and hardware limitations. Finally, we experimentally reconstruct the autocorrelation function of the effective magnetic field produced by the nuclear-spin bath on the electronic spin of a single nitrogen-vacancy center in diamond, discuss practical limitations of the method, and avenues to further improve the reconstruction accuracy.

Using a single nitrogen-vacancy center in diamond to detect microwave magnetic field vectors at resonant frequency

This study introduces a method for reconstructing vector microwave magnetic fields using a single nitrogen-vacancy (NV) center in locally strong effective fields with two different orientations in diamond, without the previously required external magnetic field. Due to the varying orientations of the effective fields, NV centers exhibit two distinct sets of switchable ground states. The resonant Rabi oscillations of an NV center in these two distinct states were utilized to reconstruct vector microwave magnetic fields. Remarkably, this technique achieves an angular resolution of 0.02 mrad/Hz. Overcoming the limitations inherent in previous practices of using NV ensembles, this breakthrough has the potential to substantially enhance both the spatial resolution and the sensitivity of microwave magnetic field imaging, a meaningful development for various scientific and technological applications.

Room Temperature Relaxometry of Single Nitrogen Vacancy Centers in Proximity to α-RuCl3 Nanoflakes.

Nitrogen vacancy (NV) center-based magnetometry has been proven to be a versatile sensor for various classes of magnetic materials in broad temperature and frequency ranges. Here, we use the longitudinal relaxation time T1 of single NV centers to investigate the spin dynamics of nanometer-thin flakes of α-RuCl3 at room temperature. We observe a significant reduction in the T1 in the presence of α-RuCl3 in the proximity of NVs, which we attribute to paramagnetic spin noise confined in the 2D hexagonal planes. Furthermore, the T1 time exhibits a monotonic increase with an applied magnetic field. We associate this trend with the alteration of the spin and charge noise in α-RuCl3 under an external magnetic field. These findings suggest that the influence of the spin dynamics of α-RuCl3 on the T1 of the NV center can be used to gain information about the material itself and the technique to be used on other 2D materials.

Suppression of Pulsed Dynamic Nuclear Polarization by Many-Body Spin Dynamics.

We study a mechanism by which nuclear hyperpolarization due to the polarization transfer from a microwave-pulse-controlled electron spin is suppressed. From analytical and numerical calculations of the unitary dynamics of multiple nuclear spins, we uncover that, combined with the formation of the dark state within a cluster of nuclei, coherent higher-order nuclear spin dynamics impose limits on the efficiency of the polarization transfer even in the absence of mundane depolarization processes such as nuclear spin diffusion and relaxation. Furthermore, we show that the influence of the dark state can be partly mitigated by introducing a disentangling operation. Our analysis is applied to the nuclear polarizations observed in ^{13}C nuclei coupled with a single nitrogen-vacancy center in diamond [Randall etal., Science 374, 1474 (2021)SCIEAS0036-807510.1126/science.abk0603]. Our Letter sheds light on collective engineering of nuclear spins as well as future designs of pulsed dynamic nuclear polarization protocols.

Mapping a 50-spin-qubit network through correlated sensing

Spins associated to optically accessible solid-state defects have emerged as a versatile platform for exploring quantum simulation, quantum sensing and quantum communication. Pioneering experiments have shown the sensing, imaging, and control of multiple nuclear spins surrounding a single electron spin defect. However, the accessible size of these spin networks has been constrained by the spectral resolution of current methods. Here, we map a network of 50 coupled spins through high-resolution correlated sensing schemes, using a single nitrogen-vacancy center in diamond. We develop concatenated double-resonance sequences that identify spin-chains through the network. These chains reveal the characteristic spin frequencies and their interconnections with high spectral resolution, and can be fused together to map out the network. Our results provide new opportunities for quantum simulations by increasing the number of available spin qubits. Additionally, our methods might find applications in nano-scale imaging of complex spin systems external to the host crystal.

Spin-State Control of Shallow Single NV Centers in Hydrogen-Terminated Diamond.

The ability to control the charge and spin states of nitrogen-vacancy (NV) centers near the diamond surface is of pivotal importance for quantum applications. Hydrogen-terminated diamond is promising for long spin coherence times and ease of controlling the charge states due to the low density of surface defects. However, it has so far been challenging to create negatively charged single NV centers with controllable spin states beneath a hydrogen-terminated surface because atmospheric adsorbates that act as acceptors induce surface holes. In this study, we optically detected the magnetic resonance of shallow single NV centers in hydrogen-terminated diamond through precise control of the nitrogen implantation fluence. Furthermore, we found that the probability of detecting the resonance was enhanced by reducing the surface acceptor density through passivation of the hydrogen-terminated surface with hexagonal boron nitride without air exposure. This control method opens up new opportunities for using NV centers in quantum applications.

Four-Order Power Reduction in Nanoscale Electron-Nuclear Double Resonance with a Nitrogen-Vacancy Center in Diamonds.

Detecting nuclear spins using single nitrogen-vacancy (NV) centers is of particular importance in nanoscale science and engineering but often suffers from the heating effect of microwave fields for spin manipulation, especially under high magnetic fields. Here, we realize an energy-efficient nanoscale nuclear-spin detection using a phase-modulation electron-nuclear double resonance scheme. The microwave field can be reduced to 1/250 of the previous requirements, and the corresponding power is over four orders lower. Meanwhile, the microwave-induced broadening to the line-width of the spectroscopy is significantly canceled, and we achieve a nuclear-spin spectrum with a resolution down to 2.1 kHz under a magnetic field at 1840 Gs. The spectral resolution can be further improved by upgrading the experimental control precision. This scheme can also be used in sensing microwave fields and can be extended to a wide range of applications in the future.

Fast coherent control of nitrogen-14 spins associated with nitrogen-vacancy centers in diamonds using dynamical decoupling

Abstract A nitrogen-vacancy (NV) center in a diamond enables the access to an electron spin, which is expected to present highly sensitive quantum sensors. Although exploiting a nitrogen nuclear spin improves the sensitivity, manipulating it using a resonant pulse requires a long gate time owing to its small gyromagnetic ratio. Another technique to control nuclear spins is a conditional rotation gate based on dynamical decoupling, which is faster but unavailable for nitrogen spins owing to the lack of transverse hyperfine coupling with the electron spin. In this study, we generated effective transverse coupling by applying a weak off-axis magnetic field. An effective coupling depends on the off-axis field; the conditional rotation gate on the nitrogen-14 spins of an NV center was demonstrated within 4.2 μs under an 1.8% off-axis field and a longitudinal field of approximately 280 mT. We estimated that a population transfer from the electron to nitrogen spins can be implemented with 8.7 μs. Our method is applicable to an ensemble of NV centers, in addition to a single NV center.

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.

Sensitivity improvement of a single-NV diamond magnetometer using a chiral waveguide.

A single nitrogen-vacancy (NV) center in diamond is utilized to perform nanoscale magnetic measurements. However, the low contrast and poor collection efficiency of spin-dependent emitted photons limited the instrument sensitivity to approximately several nT/Hz. Here, we design a diamond magnetometer based on a chiral waveguide. We numerically demonstrate that the proposed device achieves a sensitivity of 170 pT/Hz owing to near-unity contrast and efficient photon collection. We also confirm that the device sensitivity is robust against position misalignment and dipole misorientation of an NV center. The proposed approach will enable the construction of a highly-sensitive magnetometer with high spatial resolution.

Charge Stability and Charge-State-Based Spin Readout of Shallow Nitrogen-Vacancy Centers in Diamond.

Spin-based applications of the negatively charged nitrogen-vacancy (NV) center in diamonds require an efficient spin readout. One approach is the spin-to-charge conversion (SCC), relying on mapping the spin states onto the neutral (NV0) and negative (NV-) charge states followed by a subsequent charge readout. With high charge-state stability, SCC enables extended measurement times, increasing precision and minimizing noise in the readout compared to the commonly used fluorescence detection. Nanoscale sensing applications, however, require shallow NV centers within a few nanometers distance from the surface where surface related effects might degrade the NV charge state. In this article, we investigate the charge state initialization and stability of single NV centers implanted ≈5 nm below the surface of a flat diamond plate. We demonstrate the SCC protocol on four shallow NV centers suitable for nanoscale sensing, obtaining a reduced readout noise of 5-6 times the spin-projection noise limit. We investigate the general applicability of the SCC for shallow NV centers and observe a correlation between the NV charge-state stability and readout noise. Coating the diamond with glycerol improves both the charge initialization and stability. Our results reveal the influence of the surface-related charge environment on the NV charge properties and motivate further investigations to functionalize the diamond surface with glycerol or other materials for charge-state stabilization and efficient spin-state readout of shallow NV centers suitable for nanoscale sensing.

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.

Dopant-assisted stabilization of negatively charged single nitrogen-vacancy centers in phosphorus-doped diamond at low temperatures

Charge state instabilities have been a bottleneck for the implementation of solid-state spin systems and pose a major challenge to the development of spin-based quantum technologies. Here we investigate the stabilization of negatively charged nitrogen-vacancy (NV−) centers in phosphorus-doped diamond at liquid helium temperatures. Photoionization of phosphorous donors in conjunction with charge diffusion at the nanoscale enhances NV0 to NV− conversion and stabilizes the NV− charge state without the need for an additional repump laser. The phosphorus-assisted stabilization is explored and confirmed both with experiments and our theoretical model. Stable photoluminescence-excitation spectra are obtained for NV− centers created during the growth. The fluorescence is continuously recorded under resonant excitation to real-time monitor the charge state and the ionization and recombination rates are extracted from time traces. We find a linear laser power dependence of the recombination rate as opposed to the conventional quadratic dependence, which is attributed to the photo-ionization of phosphorus atoms.

High-resolution nanoscale NMR for arbitrary magnetic fields

Nitrogen vacancy (NV) centers are a major platform for the detection of nuclear magnetic resonance (NMR) signals at the nanoscale. To overcome the intrinsic electron spin lifetime limit in spectral resolution, a heterodyne detection approach is widely used. However, application of this technique at high magnetic fields is yet an unsolved problem. Here, we introduce a heterodyne detection method utilizing a series of phase coherent electron nuclear double resonance sensing blocks, thus eliminating the numerous Rabi microwave pulses required in the detection. Our detection protocol can be extended to high magnetic fields, allowing chemical shift resolution in NMR experiments. We demonstrate this principle on a weakly coupled 13C nuclear spin in the bath surrounding single NV centers, and compare the results to existing heterodyne protocols. Additionally, we identify the combination of NV-spin-initialization infidelity and strong sensor-target-coupling as linewidth-limiting decoherence source, paving the way towards high-field heterodyne NMR protocols with chemical resolution.

Single spin magnetometry and relaxometry applied to antiferromagnetic materials

Despite the considerable interest for antiferromagnets that appeared with the perspective of using them for spintronics, their experimental study, including the imaging of antiferromagnetic textures, remains a challenge. To address this issue, quantum sensors, and, in particular, the nitrogen-vacancy (NV) defects in diamond have become a widespread technical solution. We review here the recent applications of single NV centers to study a large variety of antiferromagnetic materials, from quantitative imaging of antiferromagnetic domains and non-collinear states, to the detection of spin waves confined in antiferromagnetic textures and the non-perturbative measurement of spin transport properties. We conclude with recent developments improving further the magnetic sensitivity of scanning NV microscopy, opening the way to detailed investigations of the internal texture of antiferromagnetic objects.

Temperature Dependence of Photoluminescence Intensity and Spin Contrast in Nitrogen-Vacancy Centers.

We report on measurements of the photoluminescence properties of single nitrogen-vacancy centers in diamond at temperatures between 4K and 300K. We observe a strong reduction of the PL intensity and spin contrast between ca. 10K and 100K that recovers to high levels below and above. Further, we find a rich dependence on magnetic bias field and crystal strain. We develop a comprehensive model based on spin mixing and orbital hopping in the electronic excited state that quantitatively explains the observations. Beyond a more complete understanding of the excited-state dynamics, our work provides a novel approach for probing electron-phonon interactions and a predictive tool for optimizing experimental conditions for quantum applications.

Enhancing photon collection from single shallow nitrogen-vacancy centers in diamond nanopillars for quantum heterodyne measurements

The developments in quantum sensing protocols and nano-photonic waveguides are merged to improve the performance of single nitrogen-vancancy (NV) centers in nuclear magnetic resonance (NMR) sensing. Nanopillars are designed with NV centers placed approximately 5 nm below the top facet and fabricated through a simple procedure, suitable for mass production. Fluorescence intensities from these nanopillars are 3.5 times greater than that of single shallow NV centers embedded in unstructured flat diamond. Quantum heterodyne measurements of an alternating magnetic field are performed with these nanopillars and evidence of improved peak clarity in the frequency spectrum is shown.