Nitrogen-vacancy Electron Spin Research Articles

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.

Surface optimization of nanodiamonds using non-thermal plasma

Sensitive local monitoring of intracellular processes by quantum sensing utilizing nitrogen-vacancy (NV) centers in nanodiamonds (NDs), would greatly advance cell biology and medicine. However, NDs still fall behind in sensitivity compared to bulk diamond because of their much shorter NV relaxation times. As suggested in theoretical studies, prolongation of NV relaxation times should be achievable by surface optimization creating mixed H/O surface termination consisting of hydrogen atoms, hydroxyl groups, and C–O–C ether bridges. Here we target such chemistry by employing a non-thermal plasma (NTP) in a point-to-plain discharge configuration in aqueous solution. We have devised a set of experiments with different types of nanodiamond samples (of HPHT or detonation origin and with an H- or O-terminated surface) and four working gases (air, O2, He, and H2). Using FTIR, we have found that NTP modification induces a relative increase of O–H and C–H bonds with respect to CO bonds. We have observed the biggest changes in FTIR spectra and the greatest decrease in zeta potential with oxidized NDs (both detonation and HPHT) and hydrogen as the working gas. NV electron spin relaxation times of thus modified HPHT NDs indicate an improvement of the T1 time by ∼17%–∼29% and the T2 time prolongation of 40%.

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.

Quantum sensing of local stray field environment of micron-scale magnetic disks

Local characterization of the properties and performances of miniaturized magnetic devices is a prerequisite for advancing present on-chip spintronic technologies. Utilizing nitrogen-vacancy (NV) centers in diamond, here we report quantum sensing of spin wave modes and magnetic stray field environment of patterned micrometer-scale Y3Fe5O12 (YIG) disks at the submicrometer length scale. Taking advantage of wide-field magnetometry techniques using NV ensembles, we map the spatially dependent NV electron spin resonances and Rabi oscillations in response to local variations of the stray fields emanating from a proximal YIG pattern. Our experimental data are in excellent agreement with theoretical predictions and micromagnetic simulation results, highlighting the significant opportunities offered by NV centers for probing the local magnetic properties of functional solid-state devices. The presented quantum sensing strategy may also find applications in the development of next-generation spintronic circuits with improved scalability and density.

Efficient and all-carbon electrical readout of a NV-based quantum sensor

The spin readout of an ensemble of nitrogen-vacancy (NV) centers in diamond can be realized by a photoconductive detection that is a complementary method to the optical detection of the NV electron spin magnetic resonance. Here, we implement the photoconductive detection through graphitic planar electrodes that collect the photocurrent. Graphitic electrodes are patterned using a xenon focused-ion beam on an optical-grade quality diamond crystal containing a nitrogen concentration of ∼1 ppm and a NV concentration of a few parts per billion. Resistance and current–voltage characteristics of the NV-doped diamond junction are investigated tuning the 532 nm pump beam intensity. The junction has an ohmic behavior and, under a strong bias field, we observe velocity saturation of the optically induced carriers in the diamond junction. We perform the photoconductive detection in the continuous-wave regime of the magnetic resonance of the NV centers ensemble for a magnetic field applied along the ⟨100⟩ and the ⟨111⟩ directions with a magnitude above 100 mT. This technique enables the realization of all-carbon diamond quantum sensors integrating graphitic microstructures for the electrical readout.

Coupling-selective quantum optimal control in weak-coupling NV-^{13}C system

Quantum systems are under various unwanted interactions due to their coupling with the environment. Efficient control of quantum system is essential for quantum information processing. Weak-coupling interactions are ubiquitous, and it is very difficult to suppress them using optimal control method, because the control operation is at a time scale of the coherent life time of the system. Nitrogen-vacancy (NV) center of diamond is a promising platform for quantum information processing. The ^{13}C nuclear spins in the bath are weakly coupled to the NV, rendering the manipulation extremely difficulty. Here, we report a coupling selective optimal control method that selectively suppresses unwanted weak coupling interactions and at the same time greatly prolongs the life time of the wanted quantum system. We applied our theory to a 3 qubit system consisting of one NV electron spin and two ^{13}C nuclear spins through weak-coupling with the NV center. In the experiments, the iSWAP^{dagger } gate with selective optimal quantum control is implemented in a time-span of T_{ctrl}= 170.25 mus, which is comparable to the phase decoherence time T_2= 203 mu s. The two-qubit controlled rotation gate is also completed in a strikingly 1020(80) mus, which is five times of the phase decoherence time. These results could find important applications in the NISQ era.

New constraints on exotic spin-dependent interactions with an ensemble-NV-diamond magnetometer.

Laboratory search of exotic interactions is crucial for exploring physics beyond the standard model. We report new experimental constraints on two exotic spin-dependent interactions at the micrometer scale based on ensembles of nitrogen-vacancy (NV) centers in diamond. A thin layer of NV electronic spin ensembles is synthesized as the solid-state spin quantum sensor, and a lead sphere is taken as the interacting nucleon source. Our result establishes new bounds for two types of exotic spin interactions at the micrometer scale. For an exotic parity-odd spin- and velocity-dependent interaction, improved bounds are set within the force range from 5 to 500μm. The upper limit of the corresponding coupling constant [Formula: see text] at 330μm is more than 1000-fold more stringent than the previous constraint. For the P, T-violating scalar-pseudoscalar nucleon-electron interaction, improved constraints are established within the force range from 6 to 45μm. The limit of the corresponding coupling constant [Formula: see text] is improved by more than one order of magnitude at 30μm. This work demonstrates that a solid-state NV ensemble can be a powerful platform for probing exotic spin-dependent interactions.

Room-temperature polarization of individual nuclear spins in diamond via anisotropic hyperfine coupling and coherent population trapping

We employ the electronic spin of a single nitrogen-vacancy (NV) defect in diamond to detect and control the quantum state of remote nuclear spins coupled by hyperfine interaction. More precisely, our work focuses on individual ^{13}text {C} nuclei featuring a moderate hyperfine coupling strength (sim 1 MHz) with the NV’s electron spin. Two different methods providing an efficient room-temperature polarization of these peculiar ^{13}text {C} nuclear spins are described. The first one is based on a polarization transfer from the NV electron spin to the ^{13}text {C} nucleus, which is mediated by the anisotropic component of the hyperfine interaction. The second one relies on coherent population trapping (CPT) within a Lambda -type energy-level configuration in the microwave domain, which enables to initialize the ^{13}text {C} nuclear spin in any quantum state superposition on the Bloch sphere. This CPT protocol is performed in an unusual regime for which relaxation from the excited level of the Lambda -scheme is externally triggered by optical pumping and separated in time from coherent microwave excitations. For these two polarization techniques, we investigate the impact of optical illumination on the nuclear spin polarization efficiency. This work adds new methods to the quantum toolbox used for coherent control of individual nuclear spins in diamond, which might find applications in quantum metrology.Graphical

Proposal for the search for new spin interactions at the micrometer scale using diamond quantum sensors

For decades, searches for exotic spin interactions have used increasingly-precise laboratory measurements to test various theoretical models of particle physics. However, most searches have focused on interaction length scales greater than 1 mm, corresponding to hypothetical boson masses less than 0.2 meV. Recently, quantum sensors based on Nitrogen-Vacancy (NV) centers in diamond have emerged as a promising platform to probe spin interactions at the micrometer scale, opening the door to explore new physics at this length scale. Here, we propose experiments to search for several hypothetical interactions between NV electron spins and moving masses. We focus on potential interactions involving the coupling of NV spin ensembles to both spin-polarized and unpolarized masses attached to vibrating mechanical oscillators. For each interaction, we estimate the sensitivity, identify optimal experimental conditions, and analyze potential systematic errors. Using multi-pulse quantum sensing protocols with NV spin ensembles to improve sensitivity, we project new constraints that are ~5 orders-of-magnitude improvement over previous constraints at the micrometer scale. We also identify a spin-polarized test mass, based on hyperpolarized 13C nuclear spins in a thin diamond membrane, which offers a favorable combination of high spin density and low stray magnetic fields. Our analysis is timely in light of a recent preprint (arXiv:2010.15667) reporting a surprising non-zero result of micrometer-scale spin-velocity interactions.

Quantum Fourier transform for nanoscale quantum sensing

The quantum Fourier transformation (QFT) is a key building block for a whole wealth of quantum algorithms. Despite its proven efficiency, only a few proof-of-principle demonstrations have been reported. Here we utilize QFT to enhance the performance of a quantum sensor. We implement the QFT algorithm in a hybrid quantum register consisting of a nitrogen-vacancy (NV) center electron spin and three nuclear spins. The QFT runs on the nuclear spins and serves to process the sensor—i.e., the NV electron spin signal. Specifically, we show the application of QFT for correlation spectroscopy, where the long correlation time benefits the use of the QFT in gaining maximum precision and dynamic range at the same time. We further point out the ability for demultiplexing the nuclear magnetic resonance (NMR) signals using QFT and demonstrate precision scaling with the number of used qubits. Our results mark the application of a complex quantum algorithm in sensing which is of particular interest for high dynamic range quantum sensing and nanoscale NMR spectroscopy experiments.

High-fidelity single-shot readout of single electron spin in diamond with spin-to-charge conversion

High fidelity single-shot readout of qubits is a crucial component for fault-tolerant quantum computing and scalable quantum networks. In recent years, the nitrogen-vacancy (NV) center in diamond has risen as a leading platform for the above applications. The current single-shot readout of the NV electron spin relies on resonance fluorescence method at cryogenic temperature. However, the spin-flip process interrupts the optical cycling transition, therefore, limits the readout fidelity. Here, we introduce a spin-to-charge conversion method assisted by near-infrared (NIR) light to suppress the spin-flip error. This method leverages high spin-selectivity of cryogenic resonance excitation and flexibility of photoionization. We achieve an overall fidelity > 95% for the single-shot readout of an NV center electron spin in the presence of high strain and fast spin-flip process. With further improvements, this technique has the potential to achieve spin readout fidelity exceeding the fault-tolerant threshold, and may also find applications on integrated optoelectronic devices.

Controllable and shortcut-based population transfers with a composite system of a nitrogen-vacancy electron spin and microwave photons

Optimal population transfer is of critical importance for quantum information processing. Here an efficient scheme is proposed for implementing controllable and shortcut-based population transfers with a nitrogen-vacancy (NV) electron spin and cavity photons. The electron spin is placed inside a setup of circuit quantum electrodynamics (QED). Under a suitable magnetic field bias, the ground state of electron spin constitutes an effective triplet. By means of the quantized cavity field and classical drivings, we obtain a $$\Delta $$ -configuration interaction within a composite three-state system. Based on the adjustable Rabi couplings, the shortcut-based population transfers can be performed controllably. Moreover, compared with the adiabatic counterparts, the operations assisted by counter-diabatic drivings need much shorter times and then are less susceptible to decoherence effects. Our scheme provides a promising avenue toward optimized transfer operations on NV center electron spins in circuit QED.

Spin coherence and depths of single nitrogen-vacancy centers created by ion implantation into diamond via screening masks

We characterize single nitrogen-vacancy (NV) centers created by 10-keVN+ ion implantation into diamond via thin SiO2 layers working as screening masks. Despite the relatively high acceleration energy compared with standard ones (<5keV) used to create near-surface NV centers, the screening masks modify the distribution of N+ ions to be peaked at the diamond surface [Ito et al., Appl. Phys. Lett. 110, 213105 (2017)]. We examine the relation between coherence times of the NV electronic spins and their depths, demonstrating that a large portion of NV centers are located within 10 nm from the surface, consistent with Monte Carlo simulations. The effect of the surface on the NV spin coherence time is evaluated through noise spectroscopy, surface topography, and x-ray photoelectron spectroscopy.

Robust optical readout and characterization of nuclear spin transitions in nitrogen-vacancy ensembles in diamond

Nuclear spin ensembles in diamond are promising candidates for quantum sensing applications, including rotation sensing. Here we perform a characterization of the optically detected nuclear-spin transitions associated with the 14N nuclear spin within diamond nitrogen vacancy (NV) centers. We observe nuclear-spin-dependent fluorescence with the contrast of optically detected 14N nuclear Rabi oscillations comparable to that of the NV electron spin. Using Ramsey spectroscopy, we investigate the temperature and magnetic-field dependence of the nuclear spin transitions in the 77.5-420 K and 350-675 G range, respectively. The nuclear quadrupole coupling constant Q was found to vary with temperature T yielding d|Q|/dT=-35.0(2) Hz/K at T=297 K. The temperature and magnetic field dependencies reported here are important for quantum sensing applications such as rotation sensing and potentially for applications in quantum information processing.

Nanoscale Detection of Magnon Excitations with Variable Wavevectors Through a Quantum Spin Sensor.

We report the optical detection of magnons with a broad range of wavevectors in magnetic insulator Y3Fe5O12 thin films by proximate nitrogen-vacancy (NV) single-spin sensors. Through multimagnon scattering processes, the excited magnons generate fluctuating magnetic fields at the NV electron spin resonance frequencies, which accelerate the relaxation of NV spins. By measuring the variation of the emitted spin-dependent photoluminescence of the NV centers, magnons with variable wavevectors up to ∼5 × 107 m-1 can be optically accessed, providing an alternative perspective to reveal the underlying spin behaviors in magnetic systems. Our results highlight the significant opportunities offered by NV single-spin quantum sensors in exploring nanoscale spin dynamics of emergent spintronic materials.

Principles and techniques of the quantum diamond microscope

AbstractWe provide an overview of the experimental techniques, measurement modalities, and diverse applications of the quantum diamond microscope (QDM). The QDM employs a dense layer of fluorescent nitrogen-vacancy (NV) color centers near the surface of a transparent diamond chip on which a sample of interest is placed. NV electronic spins are coherently probed with microwaves and optically initialized and read out to provide spatially resolved maps of local magnetic fields. NV fluorescence is measured simultaneously across the diamond surface, resulting in a wide-field, two-dimensional magnetic field image with adjustable spatial pixel size set by the parameters of the imaging system. NV measurement protocols are tailored for imaging of broadband and narrowband fields, from DC to GHz frequencies. Here we summarize the physical principles common to diverse implementations of the QDM and review example applications of the technology in geoscience, biology, and materials science.

Entanglement between a Diamond Spin Qubit and a Photonic Time-Bin Qubit at Telecom Wavelength.

We report on the realization and verification of quantum entanglement between a nitrogen-vacancy electron spin qubit and a telecom-band photonic qubit. First we generate entanglement between the spin qubit and a 637nm photonic time-bin qubit, followed by photonic quantum frequency conversion that transfers the entanglement to a 1588nm photon. We characterize the resulting state by correlation measurements in different bases and find a lower bound to the Bell state fidelity of ≥0.77±0.03. This result presents an important step towards extending quantum networks via optical fiber infrastructure.

Temperature dependence of the C13 hyperfine structure of the negatively charged nitrogen-vacancy center in diamond

The nitrogen-vacancy (NV) center is a well utilized system for quantum technology, in particular quantum sensing and microscopy. Fully employing the NV center's capabilities for metrology requires a strong understanding of the behavior of the NV center with respect to changing temperature. Here, we probe the NV electronic spin density as the surrounding crystal temperature changes from 10 K to 700 K by examining its $^{13}$C hyperfine interactions. These results are corroborated with \textit{ab initio} calculations and demonstrate that the change in hyperfine interaction is small and dominated by a change in the hybridization of the orbitals constituting the spin density. Thus indicating that the defect and local crystal geometry is returning towards an undistorted structure at higher temperature.

Infrared laser threshold magnetometry with a NV doped diamond intracavity etalon.

We propose a hybrid laser system consisting of a semiconductor external cavity laser associated to an intra-cavity diamond etalon doped with nitrogen-vacancy color centers. We consider laser emission tuned to the infrared absorption line that is enhanced under the magnetic field dependent nitrogen-vacancy electron spin resonance and show that this architecture leads to a compact solid-state magnetometer that can be operated at room-temperature. The sensitivity to the magnetic field limited by the photonshot-noise of the output laser beam is estimated to be less than 1pT/Hz. Unlike usual NV center infrared magnetometry, this method would not require an external frequency stabilized laser. Since the proposed system relies on the competition between the laser threshold and an intracavity absorption, such laser-based optical sensor could be easily adapted to a broad variety of sensing applications based on absorption spectroscopy.

Scalable nuclear-spin entanglement mediated by a mechanical oscillator

We propose a solid-state hybrid platform based on an array of implanted nitrogen-vacancy (NV) centers in diamond magnetically coupled to a mechanical oscillator. The mechanical oscillator and the NV electronic spins both act as a quantum bus and allow us to induce an effective long-range interaction between distant nuclear spins, relaxing the requirements on their spatial distance. The coherent nuclear spin-spin interaction, having the form of an Ising model, can be maintained in the presence of mechanical damping and spin dephasing via a pulsed dynamical decoupling of the nuclear spins in addition to the microwave driving field of the electronic spins. The present hybrid platform provides a scalable way to prepare multipartite entanglement among nuclear spins with long coherence times and can be applied to generate graph states that may be used for universal quantum computing.