Single Nitrogen-vacancy Defect Research Articles

High-resolution spectroscopy of a single nitrogen-vacancy defect at zero magnetic field

We report a study of high-resolution microwave spectroscopy of nitrogen-vacancy (NV) centers in diamond crystals at and around zero magnetic field. We observe characteristic splitting and transition imbalance of the hyperfine transitions, which originate from level anti-crossings (LACs) in the presence of a transverse effective field. We use pulsed electron spin resonance spectroscopy to measure the zero-field spectral features of single NV centers for clearly resolving such LACs. To quantitatively analyze the magnetic resonance behavior of the hyperfine spin transitions in the presence of the effective field, we present a theoretical model, which describes the transition strengths under the action of an arbitrarily polarized microwave magnetic field. Our results are of importance for the optimization of the experimental conditions for the polarization-selective microwave excitation of spin-1 systems in zero or weak magnetic fields.

Coherent rotation of a single spin via adiabatic half passage in the presence of a ferromagnetic vortex

We experimentally and numerically study possible implementations for rotations of a single nitrogen-vacancy defect spin state in proximity to a magnetic vortex core. Dynamically controlled magnetic vortex cores have been suggested as a means to provide nanoscale, rapidly-tunable magnetic fields for spin qubit addressability and control. However, driven and thermal non-equilibrium dynamics of the vortex core complicate prospects for high-fidelity gate operations. We find that the complicated profile of the driven vortex core fringe field leads to significant, but unpredictable enhancement of both Zeeman splitting and Rabi frequency. Furthermore, the gyrotropic dynamics of the vortex core lead to a complicated evolution of the spin state. We demonstrate that the fidelity of rotations can be improved using an adiabatic passage protocol in which the vortex provides an enhancement of spin splitting and Rabi frequency while unwanted vortex dynamics are suppressed.

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

Quantitative study of the response of a single NV defect in diamond to magnetic noise

The nitrogen-vacancy (NV) defect in diamond is an efficient quantum sensor of randomly fluctuating signals via relaxometry measurements. In particular, the longitudinal spin relaxation of the NV defect accelerates in the presence of magnetic noise with a spectral component at its electron spin resonance frequency. We look into this effect quantitatively by applying a calibrated and tunable magnetic noise on a single NV defect. We show that an increase of the longitudinal spin relaxation rate translates into a reduction of the photoluminescence (PL) signal emitted under continuous optical illumination, which can be explained using a simplified three-level model of the NV defect. This PL quenching mechanism offers a simple, all-optical method to detect magnetic noise sources at the nanoscale.

Imaging non-collinear antiferromagnetic textures via single spin relaxometry

Antiferromagnetic materials are promising platforms for next-generation spintronics owing to their fast dynamics and high robustness against parasitic magnetic fields. However, nanoscale imaging of the magnetic order in such materials with zero net magnetization remains a major experimental challenge. Here we show that non-collinear antiferromagnetic spin textures can be imaged by probing the magnetic noise they locally produce via thermal populations of magnons. To this end, we perform nanoscale, all-optical relaxometry with a scanning quantum sensor based on a single nitrogen-vacancy (NV) defect in diamond. Magnetic noise is detected through an increase of the spin relaxation rate of the NV defect, which results in an overall reduction of its photoluminescence signal under continuous laser illumination. As a proof-of-concept, the efficiency of the method is demonstrated by imaging various spin textures in synthetic antiferromagnets, including domain walls, spin spirals and antiferromagnetic skyrmions. This imaging procedure could be extended to a large class of intrinsic antiferromagnets and opens up new opportunities for studying the physics of localized spin wave modes for magnonics.

Spin-torque oscillation in a magnetic insulator probed by a single-spin sensor

Coherent, self-sustained oscillation of magnetization in spin-torque oscillators (STOs) is a promising source for on-chip, nanoscale generation of microwave magnetic fields. Such fields could be used for local excitation of spin-wave resonances, control of spin qubits, and studies of paramagnetic resonance. However, local characterization of fields emitted by an STO has remained an outstanding challenge. Here, we use the spin of a single nitrogen-vacancy (NV) defect in diamond to probe the magnetic fields generated by an STO in a microbar of ferromagnetic insulator yttrium-iron-garnet (YIG). The combined spectral resolution and sensitivity of the NV sensor allows us to resolve multiple spin-wave modes and characterize their damping. When damping is decreased sufficiently via spin injection, the modes auto-oscillate, as indicated by a strongly reduced linewidth, a diverging magnetic power spectral density, and synchronization of the STO frequency to an external microwave source. These results open the way for quantitative, nanoscale mapping of the microwave signals generated by STOs, as well as harnessing STOs as local probes of mesoscopic spin systems.

Microcontroller-based magnetometer using a single nitrogen-vacancy defect in a nanodiamond

The measurement of magnetic properties of various physical systems with nanometric spatial resolution raises interest in areas such as materials science, biotechnology, and information storage and processing. In the present work, a microcontroller-based magnetometer was built using a single nitrogen-vacancy defect in a nanodiamond. The implemented nanomagnetometry method is simple and relies on the frequency modulation of the nitrogen-vacancy defect electron spin resonance using square pulses of an externally applied magnetic field and employs a single microwave source. The developed system has a reasonable sensitivity of 4 μT/Hz and is able to measure magnetic field variations at a rate of around 4 mT/s. This system was used for nanoimaging the inhomogeneous spatial magnetic field profile of a magnetized steel microwire, and a spatial magnetic field gradient of 13 μT/63 nm was measured. Besides its usefulness in nanoscale imaging of magnetic fields, the present work can be of interest in the development of compact nanodiamond based magnetometers.

Laser-induced heating in a high-density ensemble of nitrogen-vacancy centers in diamond and its effects on quantum sensing

Among quantum sensors, the single nitrogen-vacancy (NV) defect in diamond has the highest sensitivity-to-size factor. For instance, a single-NV spin when used as a magnetometer could achieve sensitivities of the order of nT/Hz, while the dimensions of the sensor are merely atomic in size. The sensitivity is limited only by the photon shot noise. One method to boost the magnetometer sensitivity to pico-tesla scales is to use many NV defect centers as an ensemble sensor [Phys. Rev. X5, 041001 (2015)PRXHAE2160-330810.1103/PhysRevX.5.041001]. However, during the absorption-emission (fluorescence) optical cycles, the NV centers transfer a portion of the irradiation laser energy into phonons and heat the diamond matrix. This results in unintended fluorescence decrease, spin resonance lines shifts, and fluctuations. Hence, the advantages gained by packing a high density of NV centers are significantly reduced. Here we investigate the heat generation of ensemble NV centers in micrometer-sized diamond under 532 nm laser irradiation and its effects pertaining to sensing applications. These investigations help us to find strategies that mitigate the detrimental effects of heating and yet permits the use of ensemble NV defects for improved metrology applications.

Accurate placement of single nanoparticles on opaque conductive structures

Single quantum emitters coupled to different plasmonic and photonic structures are key elements for integrated quantum technologies. In order to fully exploit these elements, e.g., for quantum enhanced sensors or quantum repeaters, a reliable fabrication method as enabling technology is crucial. In this work, we present a method that allows for positioning of individual nanocrystals containing single quantum light sources on non-transparent conductive samples with sub-micrometer precision. We induce long-range electrostatic forces between an atomic force microscope tip, which carries a nanoparticle, and the target surface. This allows for mapping of the target area in the non-contact mode. Then, the placement site can be identified with high accuracy without any tip approach, eliminating the risk of a particle loss. We demonstrate the strength of the method by transferring a diamond nanocrystal containing a single nitrogen-vacancy defect to the center of a micrometer-sized silver bullseye antenna with nanometer resolution. Our approach provides a simple and reliable assembling technology for positioning single nano-objects on opaque substrates with high reproducibility and precision.

Coupling a Single Nitrogen-Vacancy Center in Nanodiamond to Superparamagnetic Nanoparticles

Single nitrogen-vacancy (NV) defect centers in diamond have been exploited as single photon sources and spin qubits due to their room-temperature robust quantum light emission and long electron spin coherence times. They were coupled to a manifold of structures, such as optical cavities, plasmonic waveguides, and even injected into living cells to study fundamental interactions of various nature at the nanoscale. Of particular interest are applications of NVs as quantum sensors for local nanomagnetometry. Here, we employ a nanomanipulation approach to couple a single NV center in a nanodiamond to a single few-nm superparamagnetic iron oxide nanoparticle in a controlled way. After measuring via relaxometry the magnetic particle spin-noise, we take advantage of the crystal strain ms = ± 1 spin level separation to detect the superparamagnetic particle’s effect in presence of a driving AC magnetic field. Our experiments provide detailed insight in the behavior of such particles with respect to high frequency fields. The approach can be extended to the investigation of increasingly complex, but controlled nanomagnetic hybrid particle assemblies. Moreover, our results suggest that superparamagnetic nanoparticles can amplify local magnetic interactions in order to improve the sensitivity of diamond nanosensors for specific measurement scenarios.

Strain Coupling of a Mechanical Resonator to a Single Quantum Emitter in Diamond

The recent maturation of hybrid quantum devices has led to significant enhancements in the functionality of a wide variety of quantum systems. In particular, harnessing mechanical resonators for manipulation and control has expanded the use of two-level systems in quantum information science and quantum sensing. In this letter, we report on a monolithic hybrid quantum device in which strain fields associated with resonant vibrations of a diamond cantilever dynamically control the optical transitions of a single nitrogen-vacancy (NV) defect center in diamond. We quantitatively characterize the strain coupling to the orbital states of the NV center, and with mechanical driving, we observe NV-strain couplings exceeding 10 GHz. Furthermore, we use this strain-mediated coupling to match the frequency and polarization dependence of the zero-phonon lines of two spatially separated and initially distinguishable NV centers. The experiments demonstrated here mark an important step toward engineering a quantum device capable of realizing and probing the dynamics of non-classical states of mechanical resonators, spin-systems, and photons.

Direct measurement of interfacial Dzyaloshinskii-Moriya interaction inX|CoFeB|MgOheterostructures with a scanning NV magnetometer(X=Ta,TaN, and W)

The Dzyaloshinskii-Moriya Interaction (DMI) has recently attracted considerable interest owing to its fundamental role in the stabilization of chiral spin textures in ultrathin ferromagnets, which are interesting candidates for future spintronic technologies. Here we employ a scanning nano-magnetometer based on a single nitrogen-vacancy (NV) defect in diamond to locally probe the strength of the interfacial DMI in CoFeB/MgO ultrathin films grown on different heavy metal underlayers X=Ta,TaN, and W. By measuring the stray field emanating from DWs in micron-long wires of such materials, we observe deviations from the Bloch profile for TaN and W underlayers that are consistent with a positive DMI value favoring right-handed chiral spin structures. Moreover, our measurements suggest that the DMI constant might vary locally within a single sample, illustrating the importance of local probes for the study of magnetic order at the nanoscale.

Coherent Population Trapping of a Single Nuclear Spin Under Ambient Conditions.

We demonstrate coherent population trapping of a single nuclear spin in a room-temperature solid. To this end, we exploit a three-level system with a Λ configuration in the microwave domain, which consists of nuclear spin states addressed through their hyperfine coupling to the electron spin of a single nitrogen-vacancy defect in diamond. Moreover, the Λ-scheme relaxation is externally controlled through incoherent optical pumping and separated in time from consecutive coherent microwave excitations. Such a scheme allows us (i)to monitor the sequential accumulation of population into the dark state and (ii)to reach a novel regime of coherent population trapping dynamics for which periodic arrays of dark resonances can be observed, owing to multiple constructive interferences. This Letter offers new prospects for quantum state preparation, information storage in hybrid quantum systems, and metrology.

Competition between electric field and magnetic field noise in the decoherence of a single spin in diamond

We analyze the impact of electric field and magnetic field fluctuations in the decoherence of the electronic spin associated with a single nitrogen-vacancy (NV) defect in diamond by engineering spin eigenstates protected either against magnetic noise or against electric noise. The competition between these noise sources is analyzed quantitatively by changing their relative strength through modifications of the environment. This study provides significant insights into the decoherence of the NV electronic spin, which is valuable for quantum metrology and sensing applications.

The nature of domain walls in ultrathin ferromagnets revealed by scanning nanomagnetometry.

The capacity to propagate magnetic domain walls with spin-polarized currents underpins several schemes for information storage and processing using spintronic devices. A key question involves the internal structure of the domain walls, which governs their response to certain current-driven torques such as the spin Hall effect. Here we show that magnetic microscopy based on a single nitrogen-vacancy defect in diamond can provide a direct determination of the internal wall structure in ultrathin ferromagnetic films under ambient conditions. We find pure Bloch walls in Ta/CoFeB(1 nm)/MgO, while left-handed Néel walls are observed in Pt/Co(0.6 nm)/AlOx. The latter indicates the presence of a sizable interfacial Dzyaloshinskii-Moriya interaction, which has strong bearing on the feasibility of exploiting novel chiral states such as skyrmions for information technologies.

Enhanced photoluminescence from single nitrogen-vacancy defects in nanodiamonds coated with phenol-ionic complexes.

Fluorescent nanodiamonds are attracting major attention in the field of bio-sensing and bio-labeling. In this work we demonstrate a robust approach to achieve an encapsulation of individual nanodiamonds with phenol-ionic complexes that enhance the photoluminescence from single nitrogen vacancy (NV) centers. We show that single NV centres in the coated nanodiamonds also exhibit shorter lifetimes, opening another channel for high resolution sensing. We propose that the nanodiamond encapsulation reduces the non-radiative decay pathways of the NV color centers. Our results provide a versatile and assessable way to enhance photoluminescence from nanodiamond defects that can be used in a variety of sensing and imaging applications.

Probing the dynamics of a nuclear spin bath in diamond through time-resolved central spin magnetometry.

Using fast electron spin resonance spectroscopy of a single nitrogen-vacancy defect in diamond, we demonstrate real-time readout of the Overhauser field produced by its nuclear spin environment under ambient conditions. These measurements enable narrowing the Overhauser field distribution by postselection, corresponding to a conditional preparation of the nuclear spin bath. Correlations of the Overhauser field fluctuations are quantitatively inferred by analyzing the Allan deviation over consecutive measurements. This method allows us to extract the dynamics of weakly coupled nuclear spins of the reservoir.

Stray-field imaging of magnetic vortices with a single diamond spin

Despite decades of advances in magnetic imaging, obtaining direct, quantitative information with nanometre scale spatial resolution remains an outstanding challenge. Recently, a technique has emerged that employs a single nitrogen-vacancy defect in diamond as an atomic-size magnetometer, which promises significant advances. However, the effectiveness of the technique when applied to magnetic nanostructures remains to be demonstrated. Here we use a scanning nitrogen-vacancy magnetometer to image a magnetic vortex, which is one of the most iconic objects of nanomagnetism, owing to the small size (~10 nm) of the vortex core. We report three-dimensional, vectorial and quantitative measurements of the stray magnetic field emitted by a vortex in a ferromagnetic square dot, including the detection of the vortex core. We find excellent agreement with micromagnetic simulations, both for regular vortex structures and for higher-order magnetization states. These experiments establish scanning nitrogen-vacancy magnetometry as a practical and unique tool for fundamental studies in nanomagnetism.

Spin relaxometry of single nitrogen-vacancy defects in diamond nanocrystals for magnetic noise sensing

We report an experimental study of the longitudinal relaxation time ($T_1$) of the electron spin associated with single nitrogen-vacancy (NV) defects hosted in nanodiamonds (ND). We first show that $T_1$ decreases over three orders of magnitude when the ND size is reduced from 100 to 10 nm owing to the interaction of the NV electron spin with a bath of paramagnetic centers lying on the ND surface. We next tune the magnetic environment by decorating the ND surface with Gd$^{3+}$ ions and observe an efficient $T_{1}$-quenching, which demonstrates magnetic noise sensing with a single electron spin. We estimate a sensitivity down to $\approx 14$ electron spins detected within 10 s, using a single NV defect hosted in a 10-nm-size ND. These results pave the way towards $T_1$-based nanoscale imaging of the spin density in biological samples.

Assignment of the NV0575-nm zero-phonon line in diamond to a2E-2A2transition

The time-averaged emission spectrum of single nitrogen-vacancy defects in diamond gives zero-phonon lines of both the negative charge state at 637 nm (1.945 eV) and the neutral charge state at 575 nm (2.156 eV). This occurs through photo-conversion between the two charge states. Due to strain in the diamond the zero-phonon lines are split and it is found that the splitting and polarization of the two zero-phonon lines are the same. From this observation and consideration of the electronic structure of the nitrogen-vacancy center it is concluded that the excited state of the neutral center has A2 orbital symmetry. The assignment of the 575 nm transition to a 2E - 2A2 transition has not been established previously.