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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.

Various noncollinear spin textures and magnetic phases have been predicted in twisted two-dimensional CrI$_3$ due to competing ferromagnetic (FM) and antiferromagnetic (AFM) interlayer exchange from moir\'e stacking - with potential spintronic applications even when the underlying material possesses a negligible Dzyaloshinskii-Moriya or dipole-dipole interaction. Recent measurements have shown evidence of coexisting FM and AFM layer order in small-twist-angle CrI$_3$ bilayers and double bilayers. Yet, the nature of the magnetic textures remains unresolved and possibilities for their manipulation and electrical readout are unexplored. Here, we use tunneling magnetoresistance to investigate the collective spin states of twisted double-bilayer CrI$_3$ under both out-of-plane and in-plane magnetic fields together with detailed micromagnetic simulations of domain dynamics based on magnetic circular dichroism. Our results capture hysteretic and anisotropic field evolutions of the magnetic states and we further uncover two distinct non-volatile spin textures (out-of-plane and in-plane domains) at $\approx$ 1{\deg} twist angle, with a different global tunneling resistance that can be switched by magnetic field., Comment: 18 pages, 5 figures

Fe5GeTe2 single crystals can be divided into nonquenched (NQ) and quench-cooled (QC) phases with different magnetic properties. A comprehensive understanding of the magnetic property variations in the NQ and QC phases is imperative for guiding Fe5GeTe2 towards spintronics applications; however, it remains elusive. Here, we report a real-space study on the structural and magnetic properties of these two magnetic phases using cryogenic magnetic force microscopy and scanning tunneling microscopy. The thermal history introduces disorder and order to the Fe(1) sites, resulting in the NQ and QC phases exhibiting global and broken inversion symmetry, respectively. The observed magnetic domain transitions (branching to labyrinthine) in the spin reorientation process and the distinct 3D spin textures stabilized by magnetic dipolar interaction observed in field-dependent studies allow the NQ phase to exhibit a more resilient global magnetic state. In contrast, the QC phase exhibits enhanced magnetic anisotropy, resulting in a higher TC. Meanwhile, the Dzyaloshinskii-Moriya interaction (DMI) introduced by the broken inversion symmetry causes the QC phase to exhibit a localized magnetic state: no domain transformation occurs during spin reorientation, and irregular domain states are observed in field-related studies. Our work provides an important reference for understanding the complex magnetic properties in Fe5GeTe2., Comment: 18 pages,4 figures

Fe$_3$GaTe$_2$, a recently discovered van der Waals ferromagnet, demonstrates intrinsic ferromagnetism above room temperature, necessitating a comprehensive investigation of the microscopic origins of its high Curie temperature ($\textit{T}$$_C$). In this study, we reveal the electronic structure of Fe$_3$GaTe$_2$ in its ferromagnetic ground state using angle-resolved photoemission spectroscopy and density functional theory calculations. Our results establish a consistent correspondence between the measured band structure and theoretical calculations, underscoring the significant contributions of the Heisenberg exchange interaction ($\textit{J}$$_{ex}$) and magnetic anisotropy energy to the development of the high-$\textit{T}$$_C$ ferromagnetic ordering in Fe$_3$GaTe$_2$. Intriguingly, we observe substantial modifications to these crucial driving factors through doping, which we attribute to alterations in multiple spin-splitting bands near the Fermi level. These findings provide valuable insights into the underlying electronic structure and its correlation with the emergence of high-$\textit{T}$$_C$ ferromagnetic ordering in Fe$_3$GaTe$_2$., Comment: 25 pages, 4 figures

Transition metal disulfides 4$H_{b}$-Ta(S, Se)$_{2}$ with natural heterostructure of 1${T}$- and 1${H}$-Ta(S, Se)$_{2}$ layers have became the focus of correlated materials their unique combinations of Mott physics and possible topological superconductivity. In this work, we study the upper critical fields $\mu_{0}H_{c2}$ of 4$H_{b}$-TaS$_{2}$ and 4$H_{b}$-TaS$_{1.99}$Se$_{0.01}$ single crystals systematically. Transport measurements up to 35 T show that both of ${ab}$-plane and ${c}$-axis upper critical fields ($\mu_{0}H_{c2,ab}$ and $\mu_{0}H_{c2,c}$) for 4$H_{b}$-TaS$_{2}$ and 4$H_{b}$-TaS$_{1.99}$Se$_{0.01}$ exhibit a linear temperature dependent behavior down to 0.3 K, suggesting the three-dimensional superconductivity with dominant orbital depairing mechanism in bulk 4$H_{b}$-Ta(S, Se)$_{2}$. However, the zero-temperature $\mu_{0}H_{c2,ab}$(0) for both crystals are far beyond the Pauli paramagnetic limit $\mu_{0}H{\rm_{P}}$. It could be explained by the effects of spin-momentum locking in 1$H$-Ta(S, Se)$_{2}$ layers with local inversion symmetry broken and the relatively weak intersublattice interaction between 1$H$ layers due to the existence of 1$T$ layers., Comment: 6 pages, 3 figures

Itinerant ferromagnetism at room temperature is a key ingredient for spin transport and manipulation. Here, we report the realization of nearly-room-temperature itinerant ferromagnetism in Co doped Fe5GeTe2 thin flakes. The ferromagnetic transition temperature TC (323 K - 337 K) is almost unchanged when thickness is down to 12 nm and is still about 284 K at 2 nm (bilayer thickness). Theoretical calculations further indicate that the ferromagnetism persists in monolayer Fe4CoGeTe2. In addition to the robust ferromagnetism down to the ultrathin limit, Fe4CoGeTe2 exhibits an unusual temperature- and thickness-dependent intrinsic anomalous Hall effect. We propose that it could be ascribed to the dependence of band structure on thickness that changes the Berry curvature near the Fermi energy level subtly. The nearly-room-temperature ferromagnetism and tunable anomalous Hall effect in atomically thin Fe4CoGeTe2 provide opportunities to understand the exotic transport properties of two-dimensional van der Waals magnetic materials and explore their potential applications in spintronics., Comment: 28 pages, 4 figures, 1 table

Effectively tuning magnetic state by using current is essential for novel spintronic devices. Magnetic van der Waals (vdW) materials have shown superior properties for the applications of magnetic information storage based on the efficient spin torque effect. However, for most of known vdW ferromagnets, the ferromagnetic transition temperatures lower than room temperature strongly impede their applications and the room-temperature vdW spintronic device with low energy consumption is still a long-sought goal. Here, we realize the highly efficient room-temperature nonvolatile magnetic switching by current in a single-material device based on vdW ferromagnet Fe3GaTe2. Moreover, the switching current density and power dissipation are about 300 and 60000 times smaller than conventional spin-orbit-torque devices of magnet/heavymetal heterostructures. These findings make an important progress on the applications of magnetic vdW materials in the fields of spintronics and magnetic information storage., Comment: 18 page2, 4 figures

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.

Layered {\alpha}-RuCl3 is a promising material to potentially realize the long-sought Kitaev quantum spin liquid with fractionalized excitations. While evidence of this exotic state has been reported under a modest in-plane magnetic field, such behavior is largely inconsistent with theoretical expectations of Kitaev phases emerging only in out-of-plane fields. These predicted field-induced states have been mostly out of reach due to the strong easy-plane anisotropy of bulk crystals, however. We use a combination of tunneling spectroscopy, magnetotransport, electron diffraction, and ab initio calculations to study the layer-dependent magnons, anisotropy, structure, and exchange coupling in atomically thin samples. Due to structural distortions, the sign of the average off-diagonal exchange changes in monolayer {\alpha}-RuCl3, leading to a reversal of magnetic anisotropy to easy-axis. Our work provides a new avenue to tune the magnetic interactions in {\alpha}-RuCl3 and allows theoretically predicted quantum spin liquid phases for out-of-plane fields to be more experimentally accessible.

Currently, deep learning-based visual inspection has been highly successful with the help of supervised learning methods. However, in real industrial scenarios, the scarcity of defect samples, the cost of annotation, and the lack of a priori knowledge of defects may render supervised-based methods ineffective. In recent years, unsupervised anomaly localization algorithms have become more widely used in industrial inspection tasks. This paper aims to help researchers in this field by comprehensively surveying recent achievements in unsupervised anomaly localization in industrial images using deep learning. The survey reviews more than 120 significant publications covering different aspects of anomaly localization, mainly covering various concepts, challenges, taxonomies, benchmark datasets, and quantitative performance comparisons of the methods reviewed. In reviewing the achievements to date, this paper provides detailed predictions and analysis of several future research directions. This review provides detailed technical information for researchers interested in industrial anomaly localization and who wish to apply it to the localization of anomalies in other fields., Comment: submit to IEEE TIM

The Mott insulator provides an excellent foundation for exploring a wide range of strongly correlated physical phenomena, such as high-temperature superconductivity, quantum spin liquid, and colossal magnetoresistance. A Mott insulator with the simplest degree of freedom is an ideal and highly desirable system for studying the fundamental physics of Mottness. In this study, we have unambiguously identified such an anticipated Mott insulator in a van der Waals layered compound Nb3Cl8. In the high-temperature phase, where interlayer coupling is negligible, density functional theory calculations for the monolayer of Nb3Cl8 suggest a half-filled flat band at the Fermi level, whereas angle-resolved photoemission spectroscopy experiments observe a large gap. This observation is perfectly reproduced by dynamical mean-field theory calculations considering strong electron correlations, indicating a correlation-driven Mott insulator state. Since this half-filled band derived from a single 2a1 orbital is isolated from all other bands, the monolayer of Nb3Cl8 is an ideal realization of the celebrated single-band Hubbard model. Upon decreasing the temperature, the bulk system undergoes a phase transition, where structural changes significantly enhance the interlayer coupling. This results in a bonding-antibonding splitting in the Hubbard bands, while the Mott gap remains dominant. Our discovery provides a simple and seminal model system for investigating Mott physics and other emerging correlated states., Comment: 23 pages, 4 figures, and the Supplemental Material

Moir\'e magnetism, parallel with moir\'e electronics that has led to novel correlated and topological electronic states, emerges as a new venue to design and control exotic magnetic phases in twisted magnetic two-dimensional(2D) crystals. Here, we report direct evidence of noncollinear spin texture in 2D twisted double bilayer (tDB) magnet chromium triiodide (CrI$_3$). Using magneto-optical spectroscopy in tDB CrI$_3$, we revealed the presence of a net magnetization, unexpected from the composing antiferromagnetic bilayers with compensated magnetizations, and the emergence of noncollinear spins, originated from the moir\'e exchange coupling-induced spin frustrations. Exploring the twist angle dependence, we demonstrated that both features are present in tDB CrI$_3$ with twist angles from 0.5$^o$ to 5$^o$, but are most prominent in the 1.1$^o$ tDB CrI$_3$. Focusing on the temperature dependence of the 1.1$^o$ tDB CrI$_3$, we resolved the dramatic suppression in the net magnetization onset temperature and the significant softening of noncollinear spins, as a result of the moir\'e induced frustration. Our results demonstrate the power of moir\'e superlattices in introducing novel magnetic phenomena that are absent in natural 2D magnets.

We performed high-pressure transport studies on the flat-band Kagome compounds, Pd$_3$P$_2$(S$_{1-x}$Se$_x$)$_8$ ($x$ = 0, 0.25), with a diamond anvil cell. For both compounds, the resistivity exhibits an insulating behavior with pressure up to 17 GPa. With pressure above 20 GPa, a metallic behavior is observed at high temperatures in Pd$_3$P$_2$S$_8$, and superconductivity emerges at low temperatures. The onset temperature of superconducting transition $T_{\rm C}$ rises monotonically from 2 K to 4.8 K and does not saturate with pressure up to 43 GPa. For the Se-doped compound Pd$_3$P$_2$(S$_{0.75}$Se$_{0.25}$)$_8$, the $T_{\rm C}$ is about 1.5 K higher than that of the undoped one over the whole pressure range, and reaches 6.4 K at 43 GPa. The upper critical field with field applied along the $c$ axis at typical pressures is about 50$\%$ of the Pauli limit, suggesting a 3D superconductivity. The Hall coefficient in the metallic phase is low and exhibits a peaked behavior at about 30 K, which suggests either a multi-band electronic structure or an electron correlation effect in the system., Comment: 6 pages, 5 figures

Van der Waals (vdW) magnet heterostructures have emerged as new platforms to explore exotic magnetic orders and quantum phenomena. Here, we study heterostructures of layered antiferromagnets, CrI3 and CrCl3, with perpendicular and in-plane magnetic anisotropy, respectively. Using magneto-optical Kerr effect microscopy, we demonstrate out-of-plane magnetic order in the CrCl3 layer proximal to CrI3, with ferromagnetic interfacial coupling between the two. Such an interlayer exchange field leads to higher critical temperature than that of either CrI3 or CrCl3 alone. We further demonstrate significant electric-field control of the coercivity, attributed to the naturally broken structural inversion symmetry of the heterostructure allowing unprecedented direct coupling between electric field and interfacial magnetism. These findings illustrate the opportunity to explore exotic magnetic phases and engineer spintronic devices in vdW heterostructures.

We investigate the evolutions of structural parameters, optical properties, and electronic structures of a van der Waals kagome semiconductor Pd$_{3}$P$_{2}$S$_{8}$ with Se doping. When the doping level of Se increases, the bandgaps of Pd$_{3}$P$_{2}$(S$_{1-x}$Se$_{x}$)$_{8}$ single crystals decrease gradually, accompanying with the expanded unit cells. The first-principles calculations show that there is a flat band (FB) near the Fermi level in bulk Pd$_{3}$P$_{2}$S$_{8}$. This FB mainly originates from the $d_{z^2}$-like orbitals of Pd atoms in the Pd kagome lattice, which have a finite interlayer electron hopping perpendicular to the PdS$_4$ square plane. The interlayer hopping can be reinforced with Se doping, inducing a stronger interlayer coupling via the chalcogen atoms at apical sites, which reduces the bandgap and enhances the cleavage energy. In contrast, the varnishing interlayer hopping in the two-dimensional limit results in the formation of ultra-FB in the monolayers of these compounds. The easy exfoliation and the existence of unique ultra-FB near $E_{\rm F}$ make Pd$_{3}$P$_{2}$(S$_{1-x}$Se$_{x}$)$_{8}$ a model system to explore the exotic physics of FB in 2D kagome lattice., Comment: 6 pages, 4 figures

Using polarization-resolved Raman spectroscopy, we investigate layer number, temperature, and magnetic field dependence of Raman spectra in one- to four-layer $\mathrm{CrI_{3}}$. Layer-number-dependent Raman spectra show that in the paramagnetic phase a doubly degenerated $E_{g}$ mode of monolayer $\mathrm{CrI_{3}}$ splits into one $A_{g}$ and one $B_{g}$ mode in N-layer (N > 1) $\mathrm{CrI_{3}}$ due to the monoclinic stacking. Their energy separation increases in thicker samples until an eventual saturation. Temperature-dependent measurements further show that the split modes tend to merge upon cooling but remain separated until 10 K, indicating a failed attempt of the monoclinic-to-rhombohedral structural phase transition that is present in the bulk crystal. Magnetic-field-dependent measurements reveal an additional monoclinic distortion across the magnetic-field-induced layered antiferromagnetism-to-ferromagnetism phase transition. We propose a structural change that consists of both a lateral sliding toward the rhombohedral stacking and a decrease in the interlayer distance to explain our experimental observations., Comment: The article was published in ACS Nano on June 2

Twist engineering, or the alignment of two-dimensional (2D) crystalline layers with desired orientations, has led to tremendous success in modulating the charge degree of freedom in hetero- and homo-structures, in particular, in achieving novel correlated and topological electronic phases in moir\'e electronic crystals. However, although pioneering theoretical efforts have predicted nontrivial magnetism and magnons out of twisting 2D magnets, experimental realization of twist engineering spin degree of freedom remains elusive. Here, we leverage the archetypal 2D Ising magnet chromium triiodide (CrI3) to fabricate twisted double bilayer homostructures with tunable twist angles and demonstrate the successful twist engineering of 2D magnetism in them. Using linear and circular polarization-resolved Raman spectroscopy, we identify magneto-Raman signatures of a new magnetic ground state that is sharply distinct from those in natural bilayer (2L) and four-layer (4L) CrI3. With careful magnetic field and twist angle dependence, we reveal that, for a very small twist angle (~ 0.5 degree), this emergent magnetism can be well-approximated by a weighted linear superposition of those of 2L and 4L CI3 whereas, for a relatively large twist angle (~ 5 degree), it mostly resembles that of isolated 2L CrI3. Remarkably, at an intermediate twist angle (~ 1.1 degree), its magnetism cannot be simply inferred from the 2L and 4L cases, because it lacks sharp spin-flip transitions that are present in 2L and 4L CrI3 and features a dramatic Raman circular dichroism that is absent in natural 2L and 4L ones. Our results demonstrate the possibility of designing and controlling the spin degree of freedom in 2D magnets using twist engineering.

We report the discovery of superconductivity and detailed normal-state physical properties of RbV3Sb5 single crystals with V kagome lattice. RbV3Sb5 single crystals show a superconducting transition at Tc ~ 0.92 K. Meanwhile, resistivity, magnetization and heat capacity measurements indicate that it exhibits anomalies of properties at T* ~ 102 - 103 K, possibly related to the formation of charge ordering state. When T is lower than T*, the Hall coefficient RH undergoes a drastic change and sign reversal from negative to positive, which can be partially explained by the enhanced mobility of hole-type carriers. In addition, the results of quantum oscillations show that there are some very small Fermi surfaces with low effective mass, consistent with the existence of multiple highly dispersive Dirac band near the Fermi energy level., Comment: 6 pages, 4 figures

We use a combination of polarized Raman spectroscopy experiment and model magnetism-phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet $\mathrm{CrI_3}$. We reveal a novel layered-magnetism-assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in $N$-layer $\mathrm{CrI_3}$. We resolve in data and by calculations that the 1st-order $A_g$ phonon of monolayer splits into a $N$-fold multiplet in $N$-layer $\mathrm{CrI_3}$ due to the interlayer coupling ($N$>=2) and that the phonons with the multiple show distinct magnetic field dependence because of their different layered-magnetism-phonon coupling. We further find that such a layered-magnetism-phonon coupled Raman scattering mechanism extends beyond 1st-order to higher-order multi-phonon scattering processes. Our results on magneto-Raman effect of the 1st-order phonons in the multiplet and the higher-order multi-phonons in $N$-layer $\mathrm{CrI_3}$ demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underlines the unique opportunities of new spin-phonon physics in van der Waals layered magnets., Comment: 16 pages, 4 figures + supplementary material