Stable excitons in semiconductor monolayers such as transition-metal dichalcogenides (TMDCs) enable and motivate fundamental research as well as the development of room-temperature optoelectronics applications. The newly discovered layered magnetic materials present a unique opportunity to integrate optical functionalities with magnetism. We predict that a large class of antiferromagnetic semiconducting monolayers of the MPX$_3$ family exhibit giant excitonic binding energies, making them suitable platforms for magneto-optical investigations and optospintronics applications. Indeed, our investigations, based on first principles methods combined with an effective-model Bethe-Salpeter solver, show that excitons in bare Neel-MnPS$_3$ are bound by more than 1 eV, which is twice the excitonic energies in TMDCs. In addition, the antiferromagnetic ordering of monolayer samples can be inferred indirectly using different polarization of light.
The behavior of 2-dimensional (2D) van der Waals (vdW) layered magnetic materials in the 2D limit of the few-layer thickness is an important fundamental issue for the understanding of the magnetic ordering in lower dimensions. The antiferromagnetic transition temperature TN of the Heisenberg-type 2D magnetic vdW material MnPS3 was estimated as a function of the number of layers. The antiferromagnetic transition was identified by temperature-dependent Raman spectroscopy, from the broadening of a phonon peak at 155 cm-1, accompanied by an abrupt redshift and an increase of its spectral weight. T…
Evidence for Magnon-Assisted Exciton Radiation in a Layered Antiferromagnetic Semiconductor
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University（厦门大学化学化工学院固体表面物理化学国家重点实验室）；Department of Physics, Xiamen University（厦门大学物理系）；Fujian Provincial Key Laboratory of Advanced Materials Oriented Chemical Engineering, Fujian Normal University（福建师范大学面向化学工程的先进材料福建省重点实验室）
The exchange bias (EB) effect is known as a fundamentally and technologically important magnetic property of a magnetic bilayer film. It is manifested as a horizontal shift in a magnetic hysteresis loop of a film subject to cooling in the presence of a magnetic field. The EB effect in van der Waals (vdW) heterostructures offers a novel approach for tuning the magnetic properties of the newly discovered single-layer magnets, as well as adds a new impetus to magnetic vdW heterostructures. Indeed, intriguing EB effects have recently been reported in a variety of low-dimensional vdW magnetic syste…
We have developed a sensitive cryogenic second-harmonic generation microscopy to study a van der Waals antiferromagnet MnPS$_3$. We find that long-range Néel antiferromagnetic order develops from the bulk crystal down to the bilayer, while it is absent in the monolayer. Before entering the long-range antiferromagnetic ordered phase in all samples, an upturn of the second harmonic generation below 200 K indicates the formation of the short-range order and magneto-elastic coupling. We also directly image the two antiphase (180$^{\circ}$) antiferromagnetic domains and thermally-induced domain swi…
Magnetic van der Waals (vdW) materials, including ferromagnets (FM) and antiferromagnets (AFM), have given access to the investigation of magnetism in two-dimensional (2D) limit and attracted broad interests recently. However, most of them are semiconducting or insulating and the vdW itinerant magnets, especially vdW itinerant AFM, are very rare. Here, we studied the anomalous Hall effect of a vdW itinerant magnet Fe$_5$GeTe$_2$ (F5GT) with various thicknesses down to 6.8 nm (two unit cells). Despite the robust ferromagnetic ground state in thin-layer F5GT, however, we show that the electron d…
Van der Waals (vdW) heterostructures have attracted great interest because of their rich material combinations.The discovery of two-dimensional magnets has provided a new platform for magnetic vdW heterointerfaces; however, research on magnetic vdW heterointerfaces has been limited to those with ferromagnetic surfaces. Here we report a magnetic vdW heterointerface using layered intralayer-antiferromagnetic MPSe3 (M=Mn, Fe) and monolayer transition metal dichalcogenides (TMDs). We found an anomalous upshift of the excitonic peak in monolayer TMDs below the antiferromagnetic transition temperatu…
Magnetic van der Waals (vdW) materials have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far magnetic vdW materials are mainly insulating or semiconducting, and none of them possesses a high electronic mobility - a property that is rare in layered vdW materials in general. The realization of a magnetic high-mobility vdW material would open the possibility for novel magnetic twistronic or spintronic devices. Here we report very high carrier mobility in the layered vdW antiferromagnet GdTe3. The electron mobility is beyond 60,000 cm2 V…
The advent of ferromagnetism in two-dimensional (2D) van der Waals (vdW) magnets has stimulated high interest in exploring topological magnetic textures, such as skyrmions for use in future skyrmion-based spintronic devices. To engineer skyrmions in vdW magnets by transforming Bloch-type magnetic bubbles into Néel-type skyrmions, the heterostructure of heavy metal/vdW magnetic thin film has been made to induce interfacial Dzyaloshinskii-Moriya interaction (DMI). However, the unambiguous identification of the magnetic textures inherent to vdW magnets, e.g., whether the magnetic twists (skyrmion…
Magnetic ordering in topological insulators (TI) is crucial for breaking time-reversal symmetry (TRS) and thereby opening a gap in the topological surface states (TSSs) [1-6], which is the key for realizing useful topological properties such as the quantum anomalous Hall (QAH) effect, axion insulator state and the topological magnetoelectric effect. Combining TIs with magnetic materials can be expected to yield interfaces [26-28] with unique topological and magnetic phases but such interfaces largely remain unexplored. Here, we report the discovery of a novel antiferromagnetic (AFM) Van der Wa…
In two-dimensional van der Waals (vdW) magnets, the presence of magnetic orders, strong spin-orbit coupling and asymmetry at interfaces is the key ingredient for hosting chiral spin textures. However, experimental evidences for chiral magnetism in vdW magnets remain elusive. Here we demonstrate unambiguously the formation of chiral spin textures in thin Fe3GeTe2 nanoflakes using advanced magnetic electron microscopy and first-principles calculations. Specifically, electron holography analyses reveal the spin configurations of Néel-type, zero-field-stabilized skyrmions in 20-nm-thick Fe3GeTe2 n…
Van der Waals (vdW) materials are an indispensable part of functional device technology due to their versatile physical properties and ease of exfoliating to the low-dimensional limit. Among all the compounds investigated so far, the search for magnetic vdW materials has intensified in recent years, fueled by the realization of magnetism in two dimensions (2D). However, metallic magnetic vdW systems are still uncommon. In addition, they rarely host high-mobility charge carriers, which is an essential requirement for high-speed electronic applications. Another shortcoming of 2D magnets is that …
Since the discovery of ferromagnetic two-dimensional (2D) van der Waals (vdW) crystals, significant interest on such 2D magnets has emerged, inspired by their appealing properties and integration with other 2D family for unique heterostructures. In known 2D magnets, spin-orbit coupling (SOC) stabilizes perpendicular magnetic anisotropy (PMA). Such a strong SOC could also lift the chiral degeneracy, leading to the formation of topological magnetic textures such as skyrmions through the Dzyaloshinskii-Moriya interaction (DMI). Here, we report the experimental observation of Néel-type chiral magn…
Incorporating magnetism into two dimensional (2D) van der Waals (VdW) heterostrutures is crucial for the development of functional electronic and magnetic devices. Here we show that Nb3X8 (X = Cl, Br) is a family of 2D layered trimerized kagomé magnets that are paramagnetic at high temperatures and undergo a first order phase transition on cooling to a singlet magnetic state. X-ray diffraction shows that a rearrangement of the VdW stacking accompanies the magnetic transition, with high and low temperature phases consistent with STEM images of the end members α-Nb3Cl8 and \b{eta}-Nb3Br8. The te…
We present a systematic study of the electronic and magnetic properties of two-dimensional ordered alloys, consisting of two representative hosts (MnPS$_3$ and NiPS$_3$) of transition metal phosphorus trichalcogenides doped with $3d$ elements. For both hosts our DFT+U calculations are able to qualitatively reproduce the ratios and signs of all experimentally observed magnetic couplings. The relative strength of all antiferromagnetic exchange couplings, both in MnPS$_3$ as well as in NiPS$_3$, can successfully be explained using an effective direct exchange model: they reveal that the third-nei…
Using the two-level approximation of the energy barrier, we perform extensive kinetic Monte Carlo simulations to probe the relaxation characteristics in a two-dimensional ($L^{}_x\times L^{}_y$) array of magnetic nanoparticle as a function of dipolar interaction strength $h^{}_d$, aspect ratio $A^{}_r=L^{}_y/L^{}_x$, and temperature $T$. In the case of weak dipolar interaction ($h^{}_d\approx0$) and substantial temperature, the magnetic relaxation follows the Néel Brown model as expected. Interestingly, the dipolar interaction of enough strength is found to induce antiferromagnetic coupling in…
Antiferromagnetic (AFM) van der Waals (vdW) materials provide a novel platform for synthetic AFM spintronics, in which the spin-related functionalities are derived from manipulating spin configurations between the layers. Metallic vdW antiferromagnets are expected to have several advantages over the widely-studied insulating counterparts in switching and detecting the spin states through electrical currents but have been much less explored due to the lack of suitable materials. Here, utilizing the extreme sensitivity of the vdW interlayer magnetism to material composition, we report the itiner…
The discovery of van der Waals (vdW) magnets opened up a new paradigm for condensed matter physics and spintronic technologies. However, the operations of active spintronic devices with vdW magnets are so far limited to cryogenic temperatures, inhibiting its broader practical applications. Here, for the first time, we demonstrate room temperature spin-valve devices using vdW itinerant ferromagnet Fe5GeTe2 in heterostructures with graphene. The tunnel spin polarization of the Fe5GeTe2/graphene vdW interface is detected to be significantly large ~ 45 % and negative at room temperature. Lateral s…
The weak interlayer coupling in van der Waals (vdW) magnets has confined their application to two dimensional (2D) spintronic devices. Here, we demonstrate that the interlayer coupling in a vdW magnet Fe$_3$GeTe$_2$ (FGT) can be largely modulated by a protonic gate.With the increase of the protons intercalated among vdW layers,interlayer magnetic coupling increases.Because of the existence of antiferromagnetic layers in FGT nanoflakes, the increasing interlayer magnetic coupling induces exchange bias in protonated FGT nanoflakes. Most strikingly, a rarely seen zero-field cooled (ZFC) exchange …
van der Waals (vdW) magnets are receiving ever-growing attention nowadays due to their significance in both fundamental research on low-dimensional magnetism and potential applications in spintronic devices. High crystalline quality of vdW magnets is key for maintaining intrinsic magnetic and electronic properties, especially when exfoliated down to the 2D limit. Here, ultrahigh-quality air-stable vdW CrSBr crystals are synthesized using the direct vapor-solid synthesis method. The high single crystallinity and spatial homogeneity have been thoroughly evidenced at length scales from sub-mm to …
Magnetic van der Waals (vdW) materials offer a fantastic platform to investigate and exploit rich spin configurations stabilized in reduced dimensions. One tantalizing magnetic order is the interlayer antiferromagnetism in A-type vdW antiferromagnet, which may be effectively modified by the magnetic field, stacking order and thickness scaling. However, atomically revealing the interlayer spin orientation in the vdW antiferromagnet is highly challenging, because most of the material candidates exhibit an insulating ground state or instability in ambient conditions. Here, we report the layer-dep…
XPANCEO；Moscow Center for Advanced Studies（莫斯科高等研究中心）；Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences（中国科学院福建物质结构研究所）；Quantum Science Center of Guangdong–Hong Kong–Macao Greater Bay Area (Guangdong)（粤港澳大湾区量子科学中心（广东））；University of Manchester（曼彻斯特大学）；National University of Singapore（新加坡国立大学）
The development of van der Waals (vdW) crystals and their heterostructures has created a fascinating platform for exploring optoelectronic properties in the two-dimensional (2D) limit. With the recent discovery of 2D magnets, the control of the spin degree of freedom can be integrated to realize 2D spin-optoelectronics with spontaneous time-reversal symmetry breaking. Here, we report spin photovoltaic effects in vdW heterostructures of atomically thin magnet chromium triiodide (CrI3) sandwiched by graphene contacts. In the absence of a magnetic field, the photocurrent displays a distinct depen…
2D van der Waals magnets: from fundamental physics to applications
Seoul National University（首尔大学）；Sogang University（西江大学）；Yonsei University（延世大学）；California Institute of Technology（加州理工学院）；Massachusetts Institute of Technology（麻省理工学院）
