Nanoscale Magnetic Domains in Polycrystalline Mn3Sn Films Imaged by a Scanning Single-Spin Magnetometer.

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.

Layer-Dependent Magnetism and Spin Fluctuations in Atomically Thin van der Waals Magnet CrPS4.

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 the 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 and 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.

Quantum Imaging of Magnetic Phase Transitions and Spin Fluctuations in Intrinsic Magnetic Topological Nanoflakes.

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 the magnetic phase transitions and spin fluctuations in exfoliated MnBi4Te7 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.

Strong Correlation Between Superconductivity and Ferromagnetism in an Fe-Chalcogenide Superconductor.

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, demonstrating strong correlation between superconductivity and 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.

Sensing spin wave excitations by spin defects in few-layer-thick hexagonal boron nitride.

Optically active spin defects in wide bandgap 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 [Formula: see text] 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 [Formula: see text] spin defects under various experimental conditions through optically detected magnetic resonance measurements. The off-resonant dipole interaction between YIG magnons and [Formula: see text] 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.

Observation of stacking engineered magnetic phase transitions within moiré supercells of twisted van der Waals magnets.

Recent demonstrations of moiré magnetism, featuring exotic phases with noncollinear spin order in the twisted van der Waals (vdW) magnet chromium triiodide CrI3, have highlighted the potential of twist engineering of magnetic (vdW) materials. However, the local magnetic interactions, spin dynamics, and magnetic phase transitions within and across individual moiré 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 moiré 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 Néel 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 moiré superlattices.

Local Control of a Single Nitrogen-Vacancy Center by Nanoscale Engineered Magnetic Domain Wall Motion.

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 the NV spin properties. By engineering the local magnetic field environment of an NV center via nanoscale reconfigurable domain wall motion, 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 nonvolatile magnetic memory in hybrid quantum spintronic systems.

Revealing intrinsic domains and fluctuations of moiré magnetism by a wide-field quantum microscope.

Moiré magnetism featured by stacking engineered atomic registry and lattice interactions has recently emerged as an appealing quantum state of matter at the forefront of condensed matter physics research. Nanoscale imaging of moiré 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 moiré domains of opposite magnetizations appear over arrays of moiré 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 moiré magnetism and highlight the opportunities provided by quantum spin sensors in probing microscopic spin related phenomena on two-dimensional flatland.

Wide field imaging of van der Waals ferromagnet Fe3GeTe2 by spin defects in hexagonal boron nitride.

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.

Quantum Sensing and Imaging of Spin-Orbit-Torque-Driven Spin Dynamics in the Non-Collinear Antiferromagnet Mn3 Sn.

Novel non-collinear antiferromagnets with spontaneous time-reversal symmetry breaking, non-trivial 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, nanoscale imaging of both spin-orbit-torque-induced deterministic magnetic switching and chiral spin rotation in non-collinear antiferromagnet Mn3 Sn films using nitrogen-vacancy (NV) centers are reported. Direct evidence of the off-resonance dipole-dipole coupling between the spin dynamics in Mn3 Sn and proximate NV centers is also demonstrated by 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.