Observation of unconventional chiral fermions with long Fermi arcs in CoSi.

Chirality-the geometric property of objects that do not coincide with their mirror image-is found in nature, for example, in molecules, crystals, galaxies and life forms. In quantum field theory, the chirality of a massless particle is defined by whether the directions of its spin and motion are parallel or antiparallel. Although massless chiral fermions-Weyl fermions-were predicted 90 years ago, their existence as fundamental particles has not been experimentally confirmed. However, their analogues have been observed as quasiparticles in condensed matter systems. In addition to Weyl fermions1-4, theorists have proposed a number of unconventional (that is, beyond the standard model) chiral fermions in condensed matter systems5-8, but direct experimental evidence of their existence is still lacking. Here, by using angle-resolved photoemission spectroscopy, we reveal two types of unconventional chiral fermion-spin-1 and charge-2 fermions-at the band-crossing points near the Fermi level in CoSi. The projections of these chiral fermions on the (001) surface are connected by giant Fermi arcs traversing the entire surface Brillouin zone. These chiral fermions are enforced at the centre or corner of the bulk Brillouin zone by the crystal symmetries, making CoSi a system with only one pair of chiral nodes with large separation in momentum space and extremely long surface Fermi arcs, in sharp contrast to Weyl semimetals, which have multiple pairs of Weyl nodes with small separation. Our results confirm the existence of unconventional chiral fermions and provide a platform for exploring the physical properties associated with chiral fermions.

Highly Efficient Room-Temperature Nonvolatile Magnetic Switching by Current in Fe3GaTe2 Thin Flakes.

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, the highly efficient room-temperature nonvolatile magnetic switching is realized 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/heavy-metal heterostructures. These findings make an important progress on the applications of magnetic vdW materials in the fields of spintronics and magnetic information storage.

Tunable layered-magnetism-assisted magneto-Raman effect in a two-dimensional magnet CrI3.

We used 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 CrI3 We reveal a 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 CrI3 We resolve in data and by calculations that the first-order A g phonon of the monolayer splits into an N-fold multiplet in N-layer CrI3 due to the interlayer coupling [Formula: see text] and that the phonons within the multiplet 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 first-order to higher-order multiphonon scattering processes. Our results on the magneto-Raman effect of the first-order phonons in the multiplet and the higher-order multiphonons in N-layer CrI3 demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underline the unique opportunities of spin-phonon physics in van der Waals layered magnets.

Layer-Number-Dependent Antiferromagnetic and Ferromagnetic Behavior in MnSb_{2}Te_{4}.

MnBi_{2}Te_{4}, an intrinsic magnetic topological insulator, has shown layer-number-correlated magnetic and topological phases. More interestingly, in the isostructural material MnSb_{2}Te_{4}, the antiferromagnetic (AFM) and ferromagnetic (FM) states have been both observed in the bulk counterparts, which are also predicted to be topologically nontrivial. Revealing the layer-number-dependent magnetic properties of MnSb_{2}Te_{4} down to a single septuple layer (SL) is of great significance for exploring the topological phenomena. However, this is still elusive. Here, using the polar reflective magnetic circular dichroism spectroscopy, both the A-type AFM and FM behaviors are observed and comprehensively studied in MnSb_{2}Te_{4} down to a single SL limit. In A-type AFM MnSb_{2}Te_{4} flakes, an obvious odd-even layer-number effect is observed. An additional surface spin-flop (SSF) transition occurs in even-SL flakes with the number of layers larger than 2. With the AFM linear-chain model, we identify that the even-SL flakes stabilize in a collinear state between the SSF transition and the spin-flop transition due to their appropriate energy ratio between the magnetic-field-scale anisotropy and interlayer interaction. In FM MnSb_{2}Te_{4} flakes, we observe very different magnetic behaviors with an abrupt spin-flipping transition and very small saturation fields, indicating a weakened interlayer interaction. By revealing the rich magnetic states of few-SL MnSb_{2}Te_{4} on the parameter space of the number of layers, external magnetic field, and temperature, our findings pave the way for further quantum transport studies of few-SL MnSb_{2}Te_{4}.

Evolution of interlayer and intralayer magnetism in three atomically thin chromium trihalides.

We conduct a comprehensive study of three different magnetic semiconductors, CrI3, CrBr3, and CrCl3, by incorporating both few-layer and bilayer samples in van der Waals tunnel junctions. We find that the interlayer magnetic ordering, exchange gap, magnetic anisotropy, and magnon excitations evolve systematically with changing halogen atom. By fitting to a spin wave theory that accounts for nearest-neighbor exchange interactions, we are able to further determine a simple spin Hamiltonian describing all three systems. These results extend the 2D magnetism platform to Ising, Heisenberg, and XY spin classes in a single material family. Using magneto-optical measurements, we additionally demonstrate that ferromagnetism can be stabilized down to monolayer in more isotropic CrBr3, with transition temperature still close to that of the bulk.

Tailored Tunnel Magnetoresistance Response in Three Ultrathin Chromium Trihalides.

Materials that demonstrate large magnetoresistance have attracted significant interest for many decades. Extremely large tunnel magnetoresistance (TMR) has been reported by several groups across ultrathin CrI3 by exploiting the weak antiferromagnetic coupling between adjacent layers. Here, we report a comparative study of TMR in all three chromium trihalides (CrX3, X = Cl, Br, or I) in the two-dimensional limit. As the materials exhibit different transition temperatures and interlayer magnetic ordering in the ground state, tunneling measurements allow for an easy determination of the field-temperature phase diagram for the three systems. By changing sample thickness and biasing conditions, we then demonstrate how to maximize and further tailor the TMR response at different temperatures for each material. In particular, near the magnetic transition temperature, TMR is nonsaturating up to the highest fields measured for all three compounds owing to the large, field-induced exchange coupling.

Ferromagnetic van der Waals Crystal VI3.

We report structural properties, physical properties, and the electronic structure of van der Waals (vdW) crystal VI3. Detailed analysis reveals that VI3 exhibits a structural transition from monoclinic C2/ m to rhombohedral R3̅ at Ts ≈ 79 K, similar to CrX3 (X = Cl, Br, I). Below Ts, a long-range ferromagnetic (FM) transition emerges at Tc ≈ 50 K. The local moment of V in VI3 is close to the high-spin state V3+ ion ( S = 1). Theoretical calculations suggest that VI3 may be a Mott insulator with a band gap of about 0.90 eV. In addition, VI3 has a relatively small interlayer binding energy and can be exfoliated easily down to a few layers experimentally. Therefore, VI3 is a candidate for two-dimensional FM semiconductors. It also provides a novel platform to explore 2D magnetism and vdW heterostructures in S = 1 system.

One Million Percent Tunnel Magnetoresistance in a Magnetic van der Waals Heterostructure.

We report the observation of a very large negative magnetoresistance effect in a van der Waals tunnel junction incorporating a thin magnetic semiconductor, CrI3, as the active layer. At constant voltage bias, current increases by nearly one million percent upon application of a 2 T field. The effect arises from a change between antiparallel to parallel alignment of spins across the different CrI3 layers. Our results elucidate the nature of the magnetic state in ultrathin CrI3 and present new opportunities for spintronics based on two-dimensional materials.

Near-room temperature ferromagnetism and a tunable anomalous Hall effect in atomically thin Fe4CoGeTe2.

Itinerant ferromagnetism at room temperature is a key factor for spin transport and manipulation. Here, we report the realization of near-room temperature itinerant ferromagnetism in Co doped Fe5GeTe2 thin flakes. The ferromagnetic transition temperature TC (∼323 K-337 K) is almost unchanged when the thickness is as low as 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 the band structure on thickness that changes the Berry curvature near the Fermi energy level subtly. The near-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.

Macroscopic tunneling probe of Moiré spin textures in twisted CrI3.

Various noncollinear spin textures and magnetic phases have been predicted in twisted two-dimensional CrI3 due to competing ferromagnetic (FM) and antiferromagnetic (AFM) interlayer exchange from moiré 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 CrI3 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 CrI3 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 ≈1° twist angle, with a different global tunneling resistance that can be switched by magnetic field.

Pressure-induced superconductivity at 32 K in MoB2.

Since the discovery of superconductivity in MgB2 (Tc ∼ 39 K), the search for superconductivity in related materials with similar structures or ingredients has never stopped. Although about 100 binary borides have been explored, only a few of them show superconductivity with relatively low Tc. In this work, we report the discovery of superconductivity up to 32 K, which is the highest Tc in transition-metal borides, in MoB2 under pressure. The Tc of MoB2 in the α phase can be well explained by theoretical calculations in the framework of electron-phonon coupling. Furthermore, the coupling between the d electrons of Mo and the out-of-plane Mo-phonon modes are the main driving force of the 32 K superconductivity of MoB2. Our study sheds light on the exploration of high-Tc superconductors in transition metal borides.

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.

Charge instability of topological Fermi arcs in chiral crystal CoSi.

Topological boundary states emerged at the spatial boundary between topological non-trivial and trivial phases, are usually gapless, or commonly referred as metallic states. For example, the surface state of a topological insulator is a gapless Dirac state. These metallic topological boundary states are typically well described by non-interacting fermions. However, the behavior of topological boundary states with significant electron-electron interactions, which could turn the gapless boundary states into gapped ordered states, e.g., density wave states or superconducting states, is of great interest theoretically, but is still lacking evidence experimentally. Here, we report the observation of incommensurable charge density wave (CDW) formed on the topological boundary states driven by the electron-electron interactions on the (001) surface of CoSi. The wavevector of CDW varies as the temperature changes, which coincides with the evolution of topological surface Fermi arcs with temperature. The orientation of the CDW phase is determined by the chirality of the Fermi arcs, which indicates a direct association between CDW and Fermi arcs. Our finding will stimulate the search of more interactions-driven ordered states, such as superconductivity and magnetism, on the boundaries of topological materials.

Relationship between Antisite Defects, Magnetism, and Band Topology in MnSb2Te4 Crystals with TC ≈ 40 K.

MnSb2Te4 has attracted extensive attention because of its rich and adjustable magnetic properties. Here, using a modified crystal growth method, ferrimagnetic MnSb2Te4 crystals with enhanced Curie temperature (TC) of about 40 K with dominant hole-type carriers and intrinsic anomalous Hall effect is obtained. Time- and angle-resolved photoemission spectroscopy reveals that surface states are absent in both antiferromagnetic and ferrimagnetic MnSb2Te4, implying that they have topologically trivial electronic structures. We propose that the enhancement of ferrimagnetism mainly originates from the increase of intralayer magnetic coupling caused by the decrease of Sb content at Mn sites when the decrease of Mn concentration at Sb sites would prefer the nontrival band topology. Moreover, it is known that the initial saturation moment (Mis) is sensitive to the concentrations of Mn/Sb antisite defects; thus, the Mis could be a valuable parameter to evaluate the magnetic and topological properties of MnX2nTe3n+1 (X = Bi, Sb) families.

Chirality locking charge density waves in a chiral crystal.

In Weyl semimetals, charge density wave (CDW) order can spontaneously break the chiral symmetry, gap out the Weyl nodes, and drive the material into the axion insulating phase. Investigations have however been limited since CDWs are rarely seen in Weyl semimetals. Here, using scanning tunneling microscopy/spectroscopy (STM/S), we report the discovery of a novel unidirectional CDW order on the (001) surface of chiral crystal CoSi - a unique Weyl semimetal with unconventional chiral fermions. The CDW is incommensurate with both lattice momentum and crystalline symmetry directions, and exhibits an intra unit cell π phase shift in the layer stacking direction. The tunneling spectrum shows a particle-hole asymmetric V-shaped energy gap around the Fermi level that modulates spatially with the CDW wave vector. Combined with first-principle calculations, we identify that the CDW is locked to the crystal chirality and is related by a mirror reflection between the two enantiomers of the chiral crystal. Our findings reveal a novel correlated topological quantum state in chiral CoSi crystals and raise the potential for exploring the unprecedented physical behaviors of unconventional chiral fermions.

Emergence of electric-field-tunable interfacial ferromagnetism in 2D antiferromagnet heterostructures.

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.

Frustrated ferromagnetic transition in AB-stacked honeycomb bilayer.

In two-dimensional (2D) ferromagnets, anisotropy is essential for the magnetic ordering as dictated by the Mermin-Wagner theorem. But when competing anisotropies are present, the phase transition becomes nontrivial. Here, utilizing highly sensitive susceptometry of scanning superconducting quantum interference device microscopy, we probe the spin correlations of ABC-stacked CrBr3 under zero magnetic field. We identify a plateau feature in susceptibility above the critical temperature (TC) in thick samples. It signifies a crossover regime induced by the competition between easy-plane intralayer exchange anisotropy versus uniaxial interlayer anisotropy. The evolution of the critical behavior from the bulk to 2D shows that the competition between the anisotropies is magnified in the reduced dimension. It leads to a strongly frustrated ferromagnetic transition in the bilayer with fluctuation on the order of TC, which is distinct from both the monolayer and the bulk. Our observation demonstrates unconventional 2D critical behavior on a honeycomb lattice.

Ferromagnetic-antiferromagnetic coexisting ground state and exchange bias effects in MnBi4Te7 and MnBi6Te10.

Natural superlattice structures MnBi2Te4(Bi2Te3)n (n = 1, 2, ...), in which magnetic MnBi2Te4 layers are separated by nonmagnetic Bi2Te3 layers, hold band topology, magnetism and reduced interlayer coupling, providing a promising platform for the realization of exotic topological quantum states. However, their magnetism in the two-dimensional limit, which is crucial for further exploration of quantum phenomena, remains elusive. Here, complex ferromagnetic-antiferromagnetic coexisting ground states that persist down to the 2-septuple layers limit are observed and comprehensively investigated in MnBi4Te7 (n = 1) and MnBi6Te10 (n = 2). The ubiquitous Mn-Bi site mixing modifies or even changes the sign of the subtle interlayer magnetic interactions, yielding a spatially inhomogeneous interlayer coupling. Further, a tunable exchange bias effect, arising from the coupling between the ferromagnetic and antiferromagnetic components in the ground state, is observed in MnBi2Te4(Bi2Te3)n (n = 1, 2), which provides design principles and material platforms for future spintronic devices. Our work highlights a new approach toward the fine-tuning of magnetism and paves the way for further study of quantum phenomena in MnBi2Te4(Bi2Te3)n (n = 1, 2) as well as their magnetic applications.

Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer CrI3.

Using polarization-resolved Raman spectroscopy, we investigate layer number, temperature, and magnetic field dependence of Raman spectra in one- to four-layer CrI3. Layer-number-dependent Raman spectra show that in the paramagnetic phase a doubly degenerated Eg mode of monolayer CrI3 splits into one Ag and one Bg mode in N-layer (N > 1) CrI3 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.

Magneto-Memristive Switching in a 2D Layer Antiferromagnet.

Memristive devices whose resistance can be hysteretically switched by electric field or current are intensely pursued both for fundamental interest as well as potential applications in neuromorphic computing and phase-change memory. When the underlying material exhibits additional charge or spin order, the resistive states can be directly coupled, further allowing electrical control of the collective phases. The observation of abrupt, memristive switching of tunneling current in nanoscale junctions of ultrathin CrI3 , a natural layer antiferromagnet, is reported here. The coupling to spin order enables both tuning of the resistance hysteresis by magnetic field and electric-field switching of magnetization even in multilayer samples.