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Hybrid systems consisting of multiple materials with distinct physical properties and tunable interactions provide a promising route for fulfilling transformative quantum innovations. Solid-state spin qubits and superconducting circuits stand out as leading candidates in this context due to their complementary device performance and quantum mechanical properties. Here, we report experimental integration of a single nitrogen-vacancy (NV) spin qubit and an on-chip superconducting resonator for realizing multimodal quantum applications. Specifically, we have observed superconductivity enhanced NV spin relaxation, which shows a similar Hebel-Slichter peak feature around the phase transition point. In the coherent interaction regime, we show that the superconducting resonator mode is capable of exciting NV Rabi oscillations. Taking advantage of scanning NV magnetometry, we further visualized microscopic electromagnetic behaviors of the superconducting resonator, revealing the formation and evolution of superconducting vortices at the nanoscale. Our results highlight the potential of harnessing NV centers and superconducting circuits for designing hybrid systems to advance the burgeoning quantum revolution. The current study will also open a new pathway to test and evaluate miniaturized superconducting electronics for their future design and performance improvements.

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 energyefficient 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.

Twist engineering of magnetic van der Waals (vdW) moir\'e superlattices provides an attractive way to achieve precise nanoscale control over the spin degree of freedom on two-dimensional flatland. Despite the very recent demonstrations of moir\'e magnetism featuring exotic phases with noncollinear spin order in twisted vdW magnet chromium triiodide CrI3, the local magnetic interactions, spin dynamics, and magnetic phase transitions within and across individual moir\'e supercells remain elusive. Taking advantage of a scanning single-spin magnetometry platform, here we report observation of two distinct magnetic phase transitions with separate critical temperatures within a moir\'e supercell of small-angle twisted double trilayer CrI3. By measuring temperature dependent spin fluctuations at the coexisting ferromagnetic and antiferromagnetic regions in twisted CrI3, we explicitly show that the Curie temperature of the ferromagnetic state is higher than the N\'eel temperature of the antiferromagnetic one by ~10 K. Our mean-field calculations attribute such a spatial and thermodynamic phase separation to the stacking order modulated interlayer exchange coupling at the twisted interface of the moir\'e superlattices. The presented results highlight twist engineering as a promising tuning knob to realize on-demand control of not only the nanoscale spin order of moir\'e quantum matter but also its dynamic magnetic responses, which may find relevant applications in developing transformative vdW electronic and magnetic devices.

Optically active spin defects in wide band-gap semiconductors serve as a local sensor of multiple degrees of freedom in a variety of "hard" and "soft" condensed matter systems. Taking advantage of the recent progress on quantum sensing using van der Waals (vdW) quantum materials, here we report direct measurements of spin waves excited in magnetic insulator Y3Fe5O12 (YIG) by boron vacancy $V_B^-$ spin defects contained in few-layer thick hexagonal boron nitride nanoflakes. We show that the ferromagnetic resonance and parametric spin excitations can be effectively detected by $V_B^-$ spin defects under various experimental conditions through optically detected magnetic resonance measurements. The off-resonant dipole interaction between YIG magnons and $V_B^-$ spin defects is mediated by multi-magnon scattering processes, which may find relevant applications in a range of emerging quantum sensing, computing, and metrology technologies. Our results also highlight the opportunities offered by quantum spin defects in layered two-dimensional vdW materials for investigating local spin dynamic behaviors in magnetic solid-state matters.

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 NV spin properties. By engineering the local magnetic field environment of an NV center via nanoscale reconfigurable domain wall motions, 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 non-volatile magnetic memory in hybrid quantum spintronic systems., Comment: 13 pages, 5 figures

van der Waals (vdW) magnets, an emerging family of two-dimensional (2D) materials, have received tremendous attention due to their rich fundamental physics and significant potential for cutting-edge technological applications. In contrast to the conventional bulk counterparts, vdW magnets exhibit significant tunability of local material properties, such as stacking engineered interlayer coupling and layer-number dependent magnetic and electronic interactions, which promise to deliver previously unavailable merits to develop multifunctional microelectronic devices. As a further ingredient of this emerging topic, here we report nanoscale quantum sensing and imaging of atomically thin vdW magnet chromium thiophosphate CrPS4, revealing its characteristic layer-dependent 2D static magnetism and dynamic spin fluctuations. We also show a large tunneling magnetoresistance in CrPS4-based spin filter vdW heterostructures. The excellent material stability, robust strategy against environmental degradation, in combination with tailored magnetic properties highlight the potential of CrPS4 in developing state-of-the-art 2D spintronic devices for next-generation information technologies.

Moir\'e magnetism featured by stacking engineered atomic registry and lattice interactions has recently emerged as an appealing quantum state of matter at the forefront condensed matter physics research. Nanoscale imaging of moir\'e magnets is highly desirable and serves as a prerequisite to investigate a broad range of intriguing physics underlying the interplay between topology, electronic correlations, and unconventional nanomagnetism. Here we report spin defect-based wide-field imaging of magnetic domains and spin fluctuations in twisted double trilayer (tDT) chromium triiodide CrI3. We explicitly show that intrinsic moir\'e domains of opposite magnetizations appear over arrays of moir\'e supercells in low-twist-angle tDT CrI3. In contrast, spin fluctuations measured in tDT CrI3 manifest little spatial variations on the same mesoscopic length scale due to the dominant driving force of intralayer exchange interaction. Our results enrich the current understanding of exotic magnetic phases sustained by moir\'e magnetism and highlight the opportunities provided by quantum spin sensors in probing microscopic spin related phenomena on two-dimensional flatland.

Quantum geometry - the geometry of electron Bloch wavefunctions - is central to modern condensed matter physics. Due to the quantum nature, quantum geometry has two parts, the real part quantum metric and the imaginary part Berry curvature. The studies of Berry curvature have led to countless breakthroughs, ranging from the quantum Hall effect in 2DEGs to the anomalous Hall effect (AHE) in ferromagnets. However, in contrast to Berry curvature, the quantum metric has rarely been explored. Here, we report a new nonlinear Hall effect induced by quantum metric by interfacing even-layered MnBi2Te4 (a PT-symmetric antiferromagnet (AFM)) with black phosphorus. This novel nonlinear Hall effect switches direction upon reversing the AFM spins and exhibits distinct scaling that suggests a non-dissipative nature. Like the AHE brought Berry curvature under the spotlight, our results open the door to discovering quantum metric responses. Moreover, we demonstrate that the AFM can harvest wireless electromagnetic energy via the new nonlinear Hall effect, therefore enabling intriguing applications that bridges nonlinear electronics with AFM spintronics., Comment: 19 pages, 4 figures and a Supplementary Materials with 66 pages, 4 figures and 3 tables. Originally submitted to Science on Oct. 5, 2022

Noncollinear antiferromagnets with novel magnetic orders, vanishingly small net magnetization and exotic spin related properties hold enormous promise for developing next-generation, transformative spintronic applications. A major ongoing research focus of this community is to explore, control, and harness unconventional magnetic phases of this emergent material system to deliver state-of-the-art functionalities for modern microelectronics. Here we report direct imaging of magnetic domains of polycrystalline Mn3Sn films, a prototypical noncollinear antiferromagnet, using nitrogen-vacancy-based single-spin scanning microscopy. Nanoscale evolution of local stray field patterns of Mn3Sn samples are systematically investigated in response to external driving forces, revealing the characteristic "heterogeneous" magnetic switching behaviors in polycrystalline textured Mn3Sn films. Our results contribute to a comprehensive understanding of inhomogeneous magnetic orders of noncollinear antiferromagnets, highlighting the potential of nitrogen-vacancy centers to study microscopic spin properties of a broad range of emergent condensed matter systems.

The discovery of atomic monolayer magnetic materials has stimulated intense research activities in the two-dimensional (2D) van der Waals (vdW) materials community. The field is growing rapidly and there has been a large class of 2D vdW magnetic compounds with unique properties, which provides an ideal platform to study magnetism in the atomically thin limit. In parallel, based on tunneling magnetoresistance and magneto-optical effect in 2D vdW magnets and their heterostructures, emerging concepts of spintronic and optoelectronic applications such as spin tunnel field-effect transistors and spin-filtering devices are explored. While the magnetic ground state has been extensively investigated, reliable characterization and control of spin dynamics play a crucial role in designing ultrafast spintronic devices. Ferromagnetic resonance (FMR) allows direct measurements of magnetic excitations, which provides insight into the key parameters of magnetic properties such as exchange interaction, magnetic anisotropy, gyromagnetic ratio, spin-orbit coupling, damping rate, and domain structure. In this review article, we present an overview of the essential progress in probing spin dynamics of 2D vdW magnets using FMR techniques. Given the dynamic nature of this field, we focus mainly on broadband FMR, optical FMR, and spin-torque FMR, and their applications in studying prototypical 2D vdW magnets. We conclude with the recent advances in laboratory- and synchrotron-based FMR techniques and their opportunities to broaden the horizon of research pathways into atomically thin magnets., Comment: 42 pages, 16 figures, 3 tables

Enabling scalable and energy-efficient control of spin defects in solid-state media is desirable for realizing transformative quantum information technologies. Exploiting voltage-controlled magnetic anisotropy, we report coherent manipulation of nitrogen-vacancy (NV) centers by the spatially confined magnetic stray fields produced by a proximate resonant magnetic tunnel junction (MTJ). Remarkably, the coherent coupling between NV centers and the MTJ can be systematically controlled by a DC bias voltage, allowing for appreciable electrical tunability in the presented hybrid system. In comparison with current state-of-the-art techniques, the demonstrated NV-based quantum operational platform exhibits significant advantages in scalability, device compatibility, and energy-efficiency, further expanding the role of NV centers in a broad range of quantum computing, sensing, and communications applications., Comment: 13 pages, 4 figures

Novel noncollinear antiferromagnets with spontaneous time-reversal symmetry breaking, nontrivial band topology, and unconventional transport properties have received immense research interest over the past decade due to their rich physics and enormous promise in technological applications. One of the central focuses in this emerging field is exploring the relationship between the microscopic magnetic structure and exotic material properties. Here, the nanoscale imaging of both spin-orbit-torque-induced deterministic magnetic switching and chiral spin rotation in noncollinear antiferromagnet Mn3Sn films using nitrogen-vacancy (NV) centers is reported. Direct evidence of the off-resonance dipole-dipole coupling between the spin dynamics in Mn3Sn and proximate NV centers is also demonstrated with NV relaxometry measurements. These results demonstrate the unique capabilities of NV centers in accessing the local information of the magnetic order and dynamics in these emergent quantum materials and suggest new opportunities for investigating the interplay between topology and magnetism in a broad range of topological magnets., Comment: 16 pages, 5 figures

Emergent color centers with accessible spins hosted by van der Waals materials have attracted substantial interest in recent years due to their significant potential for implementing transformative quantum sensing technologies. Hexagonal boron nitride (hBN) is naturally relevant in this context due to its remarkable ease of integration into devices consisting of low-dimensional materials. Taking advantage of boron vacancy spin defects in hBN, we report nanoscale quantum imaging of low-dimensional ferromagnetism sustained in Fe3GeTe2/hBN van der Waals heterostructures. Exploiting spin relaxometry methods, we have further observed spatially varying magnetic fluctuations in the exfoliated Fe3GeTe2 flake, whose magnitude reaches a peak value around the Curie temperature. Our results demonstrate the capability of spin defects in hBN of investigating local magnetic properties of layered materials in an accessible and precise way, which can be extended readily to a broad range of miniaturized van der Waals heterostructure systems., Comment: 13 pages, 5 figures

Topological materials featuring exotic band structures, unconventional current flow patterns, and emergent organizing principles offer attractive platforms for the development of next-generation transformative quantum electronic technologies. The family of MnBi2Te4 (Bi2Te3)n materials is naturally relevant in this context due to their nontrivial band topology, tunable magnetism, and recently discovered extraordinary quantum transport behaviors. Despite numerous pioneering studies, to date, the local magnetic properties of MnBi2Te4 (Bi2Te3)n remain an open question, hindering a comprehensive understanding of their fundamental material properties. Exploiting nitrogen-vacancy (NV) centers in diamond, we report nanoscale quantum imaging of magnetic phase transitions and spin fluctuations in exfoliated MnBi2Te4 (Bi2Te3)n flakes, revealing the underlying spin transport physics and magnetic domains at the nanoscale. Our results highlight the unique advantage of NV centers in exploring the magnetic properties of emergent quantum materials, opening new opportunities for investigating the interplay between topology and magnetism., Comment: 19 pages, 6 figures

The interplay among topology, superconductivity, and magnetism promises to bring a plethora of exotic and unintuitive behaviors in emergent quantum materials. The family of Fe-chalcogenide superconductors FeTexSe1-x are directly relevant in this context due to their intrinsic topological band structure, high-temperature superconductivity, and unconventional pairing symmetry. Despite enormous promise and expectation, the local magnetic properties of FeTexSe1-x remain largely unexplored, which prevents a comprehensive understanding of their underlying material properties. Exploiting nitrogen vacancy (NV) centers in diamond, here we report nanoscale quantum sensing and imaging of magnetic flux generated by exfoliated FeTexSe1-x flakes, providing clear evidence of superconductivity-induced ferromagnetism in FeTexSe1-x. The coexistence of superconductivity and ferromagnetism in an established topological superconductor opens up new opportunities for exploring exotic spin and charge transport phenomena in quantum materials. The demonstrated coupling between NV centers and FeTexSe1-x may also find applications in developing hybrid architectures for next-generation, solid-state-based quantum information technologies., Comment: 12 pages, 4 figures

Recently, antiferromagnets have received revived interest due to their significant potential for developing next-generation ultrafast magnetic storage. Here we report dc spin pumping by the acoustic resonant mode in a canted easy-plane antiferromagnet {\alpha}-Fe2O3 enabled by the Dzyaloshinskii-Moriya interaction. Systematic angle and frequency dependent measurements demonstrate that the observed spin pumping signals arise from resonance-induced spin injection and inverse spin Hall effect in {\alpha}-Fe2O3/metal heterostructures, mimicking the behavior of spin pumping in conventional ferromagnet/nonmagnet systems. The pure spin current nature is further corroborated by reversal of the polarity of spin pumping signals when the spin detector is switched from platinum to tungsten which has an opposite sign of the spin Hall angle. Our results highlight the potential opportunities offered by the low-frequency acoustic resonant mode in canted easy-plane antiferromagnets for developing next-generation, functional spintronic devices., Comment: 15 pages, 5 figures

Antiferromagnetic insulators (AFIs) are of significant interest due to their potential to develop next-generation spintronic devices. One major effort in this emerging field is to harness AFIs for long-range spin information communication and storage. Here, we report a non-invasive method to optically access the intrinsic spin transport properties of an archetypical AFI {\alpha}-Fe2O3 via nitrogen-vacancy (NV) quantum spin sensors. By NV relaxometry measurements, we successfully detect the time-dependent fluctuations of the longitudinal spin density of {\alpha}-Fe2O3. The observed frequency dependence of the NV relaxation rate is in agreement with a theoretical model, from which an intrinsic spin diffusion constant of {\alpha}-Fe2O3 is experimentally measured in the absence of external spin biases. Our results highlight the significant opportunity offered by NV centers in diagnosing the underlying spin transport properties in a broad range of high-frequency magnetic materials, which are challenging to access by more conventional measurement techniques.

Nitrogen vacancy (NV) centers, optically-active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. Taking advantage of these strengths, we report on NV-based local sensing of the electrically driven insulator-to-metal transition (IMT) in a proximal Mott insulator. We studied the resistive switching properties of both pristine and ion-irradiated VO2 thin film devices by performing optically detected NV electron spin resonance measurements. These measurements probe the local temperature and magnetic field in electrically biased VO2 devices, which are in agreement with the global transport measurement results. In pristine devices, the electrically-driven IMT proceeds through Joule heating up to the transition temperature while in ion-irradiated devices, the transition occurs non-thermally, well below the transition temperature. Our results provide the first direct evidence for non-thermal electrically induced IMT in a Mott insulator, highlighting the significant opportunities offered by NV quantum sensors in exploring nanoscale thermal and electrical behaviors in Mott materials.

Nitrogen vacancy (NV) centers, optically active atomic defects in diamond, have been widely applied to emerging quantum sensing, imaging, and network efforts, showing unprecedented field sensitivity and nanoscale spatial resolution. Many of these advantages derive from their excellent quantum-coherence, controllable entanglement, and high fidelity of operations, enabling opportunities to outperform the classical counterpart. Exploiting this cutting-edge quantum metrology, we report noninvasive measurement of intrinsic spin fluctuations of magnetic insulator thin films with a spontaneous out-of-plane magnetization. The measured field dependence of NV relaxation rates is well correlated to the variation of magnon density and band structure of the magnetic samples, which are challenging to access by the conventional magnetometry methods. Our results highlight the significant opportunities offered by NV centers in diagnosing the noise environment of functional magnetic elements, providing valuable information to design next-generation, high-density, and scalable spintronic devices.

Nitrogen vacancy (NV) centers, optically-active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. One of the critical challenges to develop NV-based quantum operation platforms results from the difficulty to locally address the quantum spin states of individual NV spins in a scalable, energy-efficient manner. Here, we report electrical control of the coherent spin rotation rate of a single-spin qubit in NV-magnet based hybrid quantum systems. By utilizing electrically generated spin currents, we are able to achieve efficient tuning of magnetic damping and the amplitude of the dipole fields generated by a micrometer-sized resonant magnet, enabling electrical control of the Rabi oscillation frequency of NV spins. Our results highlight the potential of NV centers in designing functional hybrid solid-state systems for next-generation quantum-information technologies. The demonstrated coupling between the NV centers and the propagating spin waves harbored by a magnetic insulator further points to the possibility to establish macroscale entanglement between distant spin qubits.

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 multi-magnon 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 x 10^7 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., Comment: https://pubs.acs.org/doi/10.1021/acs.nanolett.0c00085