2D van der Waals materials exhibiting intrinsic magnetic order have attracted enormous interest in the last few years. [1-5] However, despite much progress in the control of their magnetic properties, for example through electrostatic gating or control of the stacking order, [6-9] little is known about the mechanisms governing fundamental magnetic processes in the ultrathin limit. For instance, the extensively studied materials CrI 3 (a semiconductor) and Fe 2 GeTe 3 (a metal) are soft ferromagnets in the bulk crystal form with a remanent magnetization far below the saturation magnetization (a few percent), [10,11] but surprisingly, they become hard ferromagnets when exfoliated to a few atomic layers, with a near squareshaped hysteresis and a large coercive field of H c ≈ 0.1−1 T. [1,12-14] Since hard ferromagnetic properties are crucial to applications, especially as a building block for van der Waals magnetic heterostructures, The recent isolation of 2D van der Waals magnetic materials has uncovered rich physics that often differs from the magnetic behavior of their bulk counterparts. However, the microscopic details of fundamental processes such as the initial magnetization or domain reversal, which govern the magnetic hysteresis, remain largely unknown in the ultrathin limit. Here a widefield nitrogen-vacancy (NV) microscope is employed to directly image these processes in few-layer flakes of the magnetic semiconductor vanadium triiodide (VI 3). Complete and abrupt switching of most flakes is observed at fields H c ≈ 0.5-1 T (at 5 K) independent of thickness. The coercive field decreases as the temperature approaches the Curie temperature (T c ≈ 50 K); however, the switching remains abrupt. The initial magnetization process is then imaged, which reveals thickness-dependent domain wall depinning fields well below H c. These results point to ultrathin VI 3 being a nucleation-type hard ferromagnet, where the coercive field is set by the anisotropy-limited domain wall nucleation field. This work illustrates the power of widefield NV microscopy to investigate magnetization processes in van der Waals ferromagnets, which can be used to elucidate the origin of the hard ferromagnetic properties of other materials and explore field-and current-driven domain wall dynamics.

A dense layer of nitrogen-vacancy (NV) centers near the surface of a diamond can be interrogated in a widefield optical microscope to produce spatially resolved maps of local quantities such as magnetic field, electric field, and lattice strain, providing potentially valuable information about a sample or device placed in proximity. Since the first experimental realization of such a widefield NV microscope in 2010, the technology has seen rapid development and demonstration of applications in various areas across condensed matter physics, geoscience, and biology. This Perspective analyzes the strengths and shortcomings of widefield NV microscopy in order to identify the most promising applications and guide future development. We begin with a brief review of quantum sensing with ensembles of NV centers and the experimental implementation of widefield NV microscopy. We then compare this technology to alternative microscopy techniques commonly employed to probe magnetic materials and charge flow distributions. Current limitations in spatial resolution, measurement accuracy, magnetic sensitivity, operating conditions, and ease of use are discussed. Finally, we identify the technological advances that solve the aforementioned limitations and argue that their implementation would result in a practical, accessible, high-throughput widefield NV microscope.

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Microscopic imaging based on nitrogen-vacancy (NV) centres in diamond, a tool increasingly used for room-temperature studies of condensed matter systems, has recently been extended to cryogenic conditions. However, it remains unclear whether the technique is viable for imaging temperaturesensitive phenomena below 10 K given the inherent laser illumination requirements, especially in a widefield configuration. Here we realise a widefield NV microscope with a field of view of 100 µm and a base temperature of 4 K, and use it to image Abrikosov vortices and transport currents in a superconducting Nb film. We observe the disappearance of vortices upon increase of laser power and their clustering about hot spots upon decrease, indicating that laser powers as low as 1 mW (4 orders of magnitude below the NV saturation) are sufficient to locally quench the superconductivity of the film (Tc = 9 K). This significant local heating is confirmed by resistance measurements, which reveal the presence of large temperature gradients (several K) across the film. We then investigate the effect of such gradients on transport currents, where the current path is seen to correlate with the temperature profile even in the fully superconducting phase. In addition to highlighting the role of temperature inhomogeneities in superconductivity phenomena, this work establishes that, under sufficiently low laser power conditions, widefield NV microscopy enables imaging over mesoscopic scales down to 4 K with a submicrometer spatial resolution, providing a new platform for real-space investigations of a range of systems from topological insulators to van der Waals ferromagnets.

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Interest in van der Waals materials often stems from a desire to miniaturize existing technologies by exploiting their intrinsic layered structures to create near-atomically thin components that do not suffer from surface defects. One appealing property is an easily switchable yet robust magnetic order, which is only sparsely demonstrated in the case of in-plane anisotropy. In this work, we use widefield nitrogen-vacancy (NV) center magnetic imaging to measure the properties of individual flakes of CuCrP2S6, a multiferroic van der Waals magnet known to exhibit weak easy-plane anisotropy in the bulk. We chart the crossover between the in-plane ferromagnetism in thin flakes down to the trilayer and the bulk behavior dominated by a low-field spin-flop transition. Further, by exploiting the directional dependence of NV center magnetometry, we are able to observe an instance of a predominantly out-of-plane ferromagetic phase near zero field, in contrast with our expectation and previous experiments on the bulk material. We attribute this to the presence of surface anisotropies caused by the sample preparation process or exposure to the ambient environment, which is expected to have more general implications for a broader class of weakly anisotropic van der Waals magnets.

The widefield diamond nitrogen-vacancy (NV) microscope is a powerful instrument for imaging magnetic fields. However, a key limitation impeding its wider adoption is its complex operation, in part due to the difficulty of precisely interfacing the sensor and sample to achieve optimum spatial resolution. Here, we demonstrate a solution to this interfacing problem that is practical and reliably minimizes NV-sample standoff. We built a compact widefield NV microscope, which incorporates an integrated widefield diamond probe with full position and angular control, and developed a systematic alignment procedure based on optical interference fringes. Using this platform, we imaged an ultrathin (1 nm) magnetic film test sample and conducted a detailed study of the spatial resolution. We reproducibly achieved an estimated NV-sample standoff (and hence spatial resolution) of at most ∼2 μm across a ∼0.5 mm field of view. Guided by these results, we suggest future improvements for approaching the optical diffraction limit. This work is a step toward realizing a widefield NV microscope suitable for routine high-throughput mapping of magnetic fields.

Van der Waals (vdW) magnets are appealing candidates for realising spintronic devices that exploit current control of magnetization (e.g. switching or domain wall motion), but so far experimental demonstrations have been sparse, in part because of challenges associated with imaging the magnetization in these systems. Widefield nitrogen-vacancy (NV) microscopy allows rapid, quantitative magnetic imaging across entire vdW flakes, ideal for capturing changes in the micromagnetic structure due to an electric current. Here we use a widefield NV microscope to study the effect of current injection in thin flakes (∽10 nm) of the vdW ferromagnet Fe3GeTe2 (FGT). We first observe current-reduced coercivity on an individual domain level, where current injection in FGT causes substantial reduction in the magnetic field required to locally reverse the magnetisation. We then explore the possibility of current-induced domain-wall motion, and provide preliminary evidence for such a motion under relatively low current densities, suggesting the existence of strong current-induced torques in our devices. Our results illustrate the applicability of widefield NV microscopy to imaging spintronic phenomena in vdW magnets, highlight the possibility of efficient magnetization control by direct current injection without assistance from an adjacent conductor, and motivate further investigations of the effect of currents in FGT and other vdW magnets.