Quantitative quantum sensing with shallow electron spins, such as those hosted by nitrogen-vacancy (NV) centers in diamond, requires accurate knowledge of the spin's depth below the host material's surface. A widely used approach infers this depth from the 1H nuclear magnetic resonance (NMR) signal of immersion oil on the diamond surface that can be detected using dynamical decoupling sequences such as XY8. However, finite-width pulses make XY8 sensitive to subharmonic responses, including unwanted contributions from nearby 13C spins, and its instrument-limited spectral resolution provides only sparse sampling of the narrow 1H NMR lineshape. Here, we introduce Spin-Lock NMR as an alternative approach to single-NV depth determination. By tuning the Spin-Lock Rabi frequency to the 1H Larmor frequency, the NV probes the 1H NMR signal through the Hartmann-Hahn resonance without the harmonic ambiguities of pulsed decoupling sequences and with substantially higher instrument-limited spectral resolution. We derive a quantitative Spin-Lock NMR fit function from a Markovian master equation that directly relates the measured spectrum to the NV depth. Our approach yields NV depth estimates in excellent agreement with the established XY8-based protocol across multiple NV centers and establishes Spin-Lock NMR as a robust alternative for quantitative single-NV depth determination. To demonstrate its applicability, we employ our method to investigate the 1H nuclear spin signal that is regularly reported to be present on diamond, even in the absence of immersion oil.
Roughness-insensitive surface magnetization is an intrinsic property of magnetoelectric antiferromagnets and is today understood as a manifestation of bulk magnetoelectric multipoles. Here, we provide an experimental quantification of the crystal-facet-dependent surface magnetization in the archetypical magnetoelectric antiferromagnet Cr_{2}O_{3} and show that the data are consistent with a quadrupolar component of the bulk magnetoelectric multipolization. Using quantitative nanoscale magnetometry on lithographically defined rectangular mesas that expose 30 distinct crystallographic facets, we quantify mesa stray magnetic fields, which arise from differences between the mesa top and side-facet magnetizations. The resulting dataset supports a linear map from surface normal to surface magnetization, from which we directly infer the bulk quadrupolar component within the multipolization framework. Our work provides systematic, facet-resolved evidence of roughness-insensitive surface magnetization, including in-plane components, and delivers a quantitative route to constraining bulk multipoles from surface stray-field data. Beyond addressing the modern theory of magnetoelectric multipolization, our approach offers a generally applicable method to quantify surface magnetizations in antiferromagnetic compounds and informs the choice of crystal cuts for future spintronics devices.
Spin-defect-based quantum microscopy has recently made transformative advances in cutting-edge scientific research and technological innovation. The high sensitivity, high spatial resolution and excellent measurement modalities of quantum spin defects open up a range of opportunities at the forefront of condensed-matter physics research. Many of the advantages of this approach result from the quantum mechanical nature of the sensors, which offer functionalities that are not available with their classical counterparts. In this Review, we provide an overview of progress on scanning-probe nitrogen-vacancy quantum sensing research and its application to investigating the physics of emergent quantum materials with nanoscale spatial resolution. We also discuss quantum sensing platforms built on more recently discovered spin defects in one-dimensional and two-dimensional materials beyond nitrogen-vacancy centres. We conclude with an outlook on future directions and opportunities for these rapidly advancing quantum sensing technologies.
Magnetic textures are central to emerging spintronic and unconventional computing technologies due to their rich dynamics, topological properties and nanoscale dimensions. A major challenge remains achieving tunable, reversible, and spatially resolved control over these textures and their evolution as a function of external stimuli, by spatially reprogramming the magnetic energy landscape that governs their nucleation and stability. Here, we exploit a focused laser-assisted local field cooling technique that establishes a fast, non-contact and scalable platform for grayscale spin texture engineering. By non-destructively controlling the exchange-bias anisotropy with nanoscale resolution in thin-film heterostructures, this approach enables grayscale, reprogrammable control of the local energy profile, which we use to create magnetic patterns with highly controlled hysteresis, field-dependent readability and tunable switching thresholds. Leveraging this capability, we demonstrate information encoding with magnetic field-gated readability, and artificial spin metamaterials, stabilizing spin lattices with field-reconfigurable symmetries and creating artificial Moiré spin textures via the geometric superposition of twisted magnetic potentials. These results establish a versatile, reprogrammable platform that bridges the gap between application-oriented magnetic memory and fundamental studies of emergent order in artificial lattices.
Spatial imaging of magnetic stray fields from magnetic materials is a useful tool for identifying the underlying magnetic configurations of the material. However, transforming the magnetic image into a magnetization image is an ill-poised problem, which can result in artefacts that limit the inferences that can be made on the material under investigation. In this work, we develop a neural network fitting approach that approximates this transformation, reducing these artefacts. Additionally, we demonstrate that this approach allows the inclusion of additional models and bounds that are not possible with traditional reconstruction methods. These advantages allow for the reconstruction of non-trivial magnetization textures with varying magnetization directions in thin-film magnets, which was not possible previously. We demonstrate this new capability by performing magnetization reconstructions on a variety of topological spin textures.
Antiferromagnetic spin textures, compared to their ferromagnetic counterparts, innately possess high stability with respect to external disturbance and high-frequency dynamics compatible with ultrafast information processing. However, deterministic creation and reconfigurable switching of different antiferromagnetic spin textures have not been realized. Here, we demonstrate room-temperature deterministic switching between three antiferromagnetic textures identified by characteristically different high frequency dynamics in single-crystal hematite (α-Fe2O3). All three states are found to be remarkably stable and fully controllable, as confirmed by 1000 switching cycles and spatially resolved spectroscopy and they may be created by local magnetization switching in the nonlinear excitation regime. The switching to the following stable state requires only one microwave pulse (100 ns) with ultralow energy consumption (1 nJ). Our Brillouin light scattering (BLS) microscopy data reinforces that the detected magnon modes are associated to excitations of domain walls and circular spin textures. The progressive switching between the three distinct states imitates the weighted sum operation in neuromorphic computing, suggesting the possibility of using spin textures in antiferromagnets for information processing.
Abstract We present a study on nanoscale skyrmionic spin textures in $$\hbox {NdMn}_{{2}}\hbox {Ge}_{{2}}$$ , a rare-earth complex noncollinear ferromagnet. We confirm, using X-ray microscopy, that $$\hbox {NdMn}_{{2}}\hbox {Ge}_{{2}}$$ can host lattices of metastable skyrmion bubbles at room temperature in the absence of a magnetic field, after applying a suitable field cooling protocol. The skyrmion bubbles are robust against temperature changes from room temperature to 330 K. Furthermore, the skyrmion bubbles can be distorted, deformed, and recovered by varying strength and orientation of the applied magnetic field. We have used nitrogen-vacancy nanoscale magnetic imaging to estimate and map the magnetic stray fields originating from our $$\hbox {NdMn}_{{2}}\hbox {Ge}_{{2}}$$ lamella samples and find stray field magnitudes on the order of a few mT near the sample surface. Micromagnetic simulations show an overall agreement with the observed behaviour of the sample under different magnetic field protocols. We also find that the presence of the Dzyaloshinskii-Moriya interaction is not required to reproduce our experimental results. Its inclusion in the simulation leads to a reversal of the skyrmionic object core polarity, which is not experimentally observed. Our results further corroborate the stability and robustness of the skyrmion bubbles formed in $${\hbox {NdMn}_2\hbox {Ge}_2}$$ and their potential for future spintronic applications.
Color center spins in diamond nanostructures are a key resource for emerging quantum technologies. Their innate surface proximity makes precise control of diamond surface chemistry essential for optimizing their functionality and charge states. However, conventional surface functionalization methods typically lack the tunability and efficiency required for robust charge-state control. Here, we introduce a deterministic, nonvolatile technique for continuously and efficiently tuning diamond's surface termination via laser-induced oxidation of H-terminated diamond nanopillars. By tracking SiV$^-$ photoluminescence as a charge-state proxy, we uncover the microscopic mechanism of this photocatalytic process through a systematic photon-flux and -energy analysis, where we identify charge-cycling of native defects as sources of optically generated holes driving the desired surface oxidation. Our results suggest that our method applies broadly to other color centers and host materials, offering a versatile tool for on-demand charge-state control and surface engineering in solid-state quantum devices.
We present in situ tuning of both the absolute and relative frequency spacing of the modes in an optical microcavity by incorporating a wedged diamond membrane. We demonstrate THz continuous tuning of doubly-resonant Raman scattering.
Quantum devices based on optically addressable spin qubits in diamond are promising platforms for quantum technologies such as quantum sensing and communication. Nano- and microstructuring of the diamond crystal is essential to enhance device performance, yet fabrication remains challenging and often involves trade-offs in surface quality, aspect ratio, device size, and uniformity. We tackle this hurdle with an approach producing millimeter-scale, thin (down to 70 nm), and highly parallel (< 0.35 nm/μm) membranes from single-crystal diamond. The membranes remain contamination free and possess atomically smooth surfaces (Rq < 200 pm) as required by state-of-the-art quantum applications. We demonstrate the benefits and versatility of our method by fabricating large fields of free-standing and homogeneous photonic nano- and microstructures. Leveraging a refined photolithography-based strategy, our method offers enhanced scalability and produces robust structures suitable for direct use, while remaining compatible with heterogeneous integration through pick-and-place transfer techniques.
Antiferromagnetic (AF) van der Waals (vdW) magnets combine the advantages of vdW magnets with the functionality of AF spintronics, offering unique opportunities for ultrafast and robust spintronic devices. However, the lack of approaches to locally and deterministically manipulate their order parameter, the Néel-vector, remains a key limitation. Here, we achieve Néel vector control in bilayers of the vdW AF CrSBr, via an effect we term lateral exchange bias (LEB). We exploit the single-crystalline registry formed by terraced CrSBr samples, where the bilayer Néel vector is controlled by LEB from neighboring, odd-layered flakes, whose nonzero magnetization we manipulate using magnetic fields. Using this control, we achieve non-volatile manipulation of magnetic domains and domain walls in AF CrSBr bilayers, establishing a powerful toolkit for controlling atomically thin AFs at the nanoscale. Our results challenge conventional views on exchange bias and provide a previously unexplored mechanism for achieving atomic-scale control of AF order. Our findings pave the way for the development of advanced spintronic architectures and quantum technologies based on vdW magnets.
Efficiently coupling a narrow-linewidth nitrogen-vacancy center (NV) in diamond to an open optical microcavity, we observe for the first time NV resonance fluorescence without requiring any time-filtering, marking a breakthrough toward high-efficiency spin-photon entanglement sources.
Two-dimensional materials are extraordinarily sensitive to external stimuli, making them ideal for studying fundamental properties and for engineering devices with new functionalities. One such stimulus, strain, affects the magnetic properties of the layered magnetic semiconductor CrSBr to such a degree that it can induce a reversible antiferromagnetic-to-ferromagnetic phase transition. Using scanning SQUID-on-lever microscopy, we directly image the effects of spatially inhomogeneous strain on the magnetization of layered CrSBr, as it is polarized by a field applied along its easy axis. The evolution of this magnetization and the formation of domains is reproduced by a micromagnetic model, which incorporates the spatially varying strain and the corresponding changes in the local interlayer exchange stiffness. The observed sensitivity to small strain gradients along with similar images of a nominally unstrained CrSBr sample suggest that unintentional strain inhomogeneity influences the magnetic behavior of exfoliated samples.
Considering the growing interest in magnetic materials for unconventional computing, data storage, and sensor applications, there is active research not only on material synthesis but also characterisation of their properties. In addition to structural and integral magnetic characterisations, imaging of magnetisation patterns, current distributions and magnetic fields at nano- and microscale is of major importance to understand the material responses and qualify them for specific applications. In this roadmap, we aim to cover a broad portfolio of techniques to perform nano- and microscale magnetic imaging using superconducting quantum interference devices, spin centre and Hall effect magnetometries, scanning probe microscopies, x-ray- and electron-based methods as well as magnetooptics and nanoscale magnetic resonance imaging. The roadmap is aimed as a single access point of information for experts in the field as well as the young generation of students outlining prospects of the development of magnetic imaging technologies for the upcoming decade with a focus on physics, materials science, and chemistry of planar, three-dimensional and geometrically curved objects of different material classes including two-dimensional materials, complex oxides, semi-metals, multiferroics, skyrmions, antiferromagnets, frustrated magnets, magnetic molecules/nanoparticles, ionic conductors, superconductors, spintronic and spinorbitronic materials.
Since their first observation in 2017, atomically thin van der Waals (vdW) magnets have attracted significant fundamental, and application-driven attention. However, their low ordering temperatures, Tc, sensitivity to atmospheric conditions and difficulties in preparing clean large-area samples still present major limitations to further progress, especially amongst van der Waals magnetic semiconductors. The remarkably stable, high-Tc vdW magnet CrSBr has the potential to overcome these key shortcomings, but its nanoscale properties and rich magnetic phase diagram remain poorly understood. Here we use single spin magnetometry to quantitatively characterise saturation magnetization, magnetic anisotropy constants, and magnetic phase transitions in few-layer CrSBr by direct magnetic imaging. We show pristine magnetic phases, devoid of defects on micron length-scales, and demonstrate remarkable air-stability down the monolayer limit. We furthermore address the spin-flip transition in bilayer CrSBr by imaging the phase-coexistence of regions of antiferromagnetically (AFM) ordered and fully aligned spins. Our work will enable the engineering of exotic electronic and magnetic phases in CrSBr and the realization of novel nanomagnetic devices based on this highly promising vdW magnet.
Magnetic random access memory (MRAM) is a leading emergent memory technology that is poised to replace current non-volatile memory technologies such as eFlash. However, the scaling of MRAM technologies is heavily affected by device-to-device variability rooted in the stochastic nature of the MRAM writing process into nanoscale magnetic layers. Here, we introduce a non-contact metrology technique deploying Scanning NV Magnetometry (SNVM) to investigate MRAM performance at the individual bit level. We demonstrate magnetic reversal characterization in individual, < 60 nm sized bits, to extract key magnetic properties, thermal stability, and switching statistics, and thereby gauge bit-to-bit uniformity. We showcase the performance of our method by benchmarking two distinct bit etching processes immediately after pattern formation. Unlike previous methods, our approach unveils marked differences in switching behaviour of fully contacted MRAM devices stemming from these processes. Our findings highlight the potential of nanoscale quantum sensing of MRAM devices for early-stage screening in the processing line, paving the way for future incorporation of this nanoscale characterization tool in the semiconductor industry.
The negatively charged boron vacancy (V-B ) center in hexagonal boron nitride (hBN) is currently garnering considerable attention for the design of two-dimensional (2D) quantum sensing units. Such developments require a precise understanding of the spin-dependent optical response of V-B centers, which still remains poorly documented despite its key role for sensing applications. Here we investigate the spin-dependent photodynamics of V-B centers in hBN by a series of time-resolved photoluminescence (PL) measurements. We first introduce a robust all-optical method to infer the spin-dependent lifetime of the excited states and the electron spin polarization of V-B centers under optical pumping. Using these results, we then analyze PL time traces recorded at different optical excitation powers with a seven-level model of the V-B center and we extract all the rates involved in the spin-dependent optical cycles, both under ambient conditions and at liquid helium temperature. These findings are finally used to study the impact of a vector magnetic field on the optical response. More precisely, we analyze PL quenching effects resulting from electron spin mixing induced by the magnetic field component perpendicular to the V-B quantization axis. All experimental results are well reproduced by the seven-level model, illustrating its robustness to describe the spin-dependent photodynamics of V-B centers. This work provides important insights into the properties of V-B centers in hBN, which are valuable for future developments of 2D quantum sensing units.
Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton coupling, and exhibiting peculiar magneto-optics of exciton-polaritons. Here, we demonstrate that both exciton and magnetic transitions in bilayer and trilayer CrSBr are sensitive to voltage-controlled field-effect charging, exhibiting bound exciton-charge complexes and doping-induced metamagnetic transitions. Moreover, we demonstrate how these unique properties enable optical probes of local magnetic order, visualizing magnetic domains of competing phases across metamagnetic transitions induced by magnetic field or electrostatic doping. Our work identifies few-layer CrSBr as a rich platform for exploring collaborative effects of charge, optical excitations, and magnetism.
Magnetism of oxide antiferromagnets (AFMs) has been studied in single crystals and extended thin films. The properties of AFM nanostructures still remain underexplored. Here, we report on the fabrication and magnetic imaging of granular 100 nm-thick magnetoelectric Cr2O3 films patterned in circular bits with diameters ranging from 500 down to 100 nm. With the change of the lateral size, the domain structure evolves from a multidomain state for larger bits to a single domain state for the smallest bits. Based on spin-lattice simulations, we show that the physics of the domain pattern formation in granular AFM bits is primarily determined by the energy dissipation upon cooling, which results in motion and expelling of AFM domain walls of the bit. Our results provide a way toward the fabrication of single domain AFM-bit-patterned memory devices and the exploration of the interplay between AFM nanostructures and their geometric shape.
Josephson junctions enable dissipation-less electrical current through metals and insulators below a critical current. Despite being central to quantum technology based on superconducting quantum bits and fundamental research into self-conjugate quasiparticles, the spatial distribution of super current flow at the junction and its predicted evolution with current bias and external magnetic field remain experimentally elusive. Revealing the hidden current flow, featureless in electrical resistance, helps understanding unconventional phenomena such as the nonreciprocal critical current, i.e., Josephson diode effect. Here we introduce a platform to visualize super current flow at the nanoscale. Utilizing a scanning magnetometer based on nitrogen vacancy centers in diamond, we uncover competing ground states electrically switchable within the zero-resistance regime. The competition results from the superconducting phase re-configuration induced by the Josephson current and kinetic inductance of thin-film superconductors. We further identify a new mechanism for the Josephson diode effect involving the Josephson current-induced phase. The nanoscale super current flow emerges as a new experimental observable for elucidating unconventional superconductivity, and optimizing quantum computation and energy-efficient devices.