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Abstract 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. 

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. 

Abstract 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 Fe₃GeTe₂flake, 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. 

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.