We investigate magnetic domain walls in a single fcc Mn layer on Re(0001) employing spin-polarized STM, atom manipulation, and spin dynamics simulations. The low symmetry of the row-wise antiferromagnetic (1Q) state leads to a new type of domain wall which connects rotational 1Q domains by a transient 2Q state with characteristic 90$^\circ$ angles between neighboring magnetic moments. The domain wall properties depend on their orientation and their width of about 2 nm essentially results from a balance of Heisenberg and higher-order exchange interactions. Atom manipulation allows domain wall imaging with atomic spin-resolution, as well as domain wall positioning, and we demonstrate that the force to move an atom is anisotropic on the 1Q domain.
Anomalous valley Hall (AVH) effect is a fundamental transport phenomenon in the field of condensed-matter physics. Usually, the research on AVH effect is mainly focused on 2D lattices with ferromagnetic order. Here, by means of model analysis, we present a general design principle for realizing AVH effect in antiferromagnetic monolayers, which involves the introduction of nonequilibrium potentials to break of PT symmetry. Using first-principles calculations, we further demonstrate this design principle by stacking antiferromagnetic monolayer MnPSe3 on ferroelectric monolayer Sc2CO2 and achieve…
How a certain ground state of complex physical systems emerges, especially in two-dimensional materials, is a fundamental question in condensed-matter physics. A particularly interesting case is systems belonging to the class of XY Hamiltonian where the magnetic order parameter of conventional nature is unstable in two-dimensional materials leading to a Berezinskii-Kosterlitz-Thouless transition. Here, we report how the XXZ-type antiferromagnetic order of a magnetic van der Waals material, NiPS3, behaves upon reducing the thickness and ultimately becomes unstable in the monolayer limit. Our ex…
The Kekule pattern of the (anti)ferromagnetic exchange field on monolayer MoS2 can be induced by proximity to the (111) surface of BiFeO3 on both sides. The three-band tight binding model of the MoS2 layer with Kekule patterned exchange field is applied to describe the heterostructures. The tight binding model is justified by the first principle calculations. The magnetization orientations of the substrates control the pattern of the exchange field, which then switches the band structures of the lowest zigzag edge states between being metallic and insulating. The lowest four zigzag edge bands …
We study the electronic properties of the heterobilayer of vanadium and iron oxychlorides, VOCl and FeOCl, two layered air stable van der Waals insulating oxides with different types of antiferromagnetic order in bulk: VOCl monolayers are ferromagnetic (FM) whereas the FeOCl monolayers are antiferromagnetic (AF). We use density functional theory (DFT) calculations, with Hubbard correction that is found to be needed to describe correctly the insulating nature of these compounds. We compute the magnetic anisotropy and propose a spin model Hamiltonian. Our calculations show that interlayer coupli…
By means of the first-principles calculations and magnetic topological quantum chemistry, we demonstrate that the low energy physics in the checkerboard antiferromagnetic (AFM) monolayer FeSe, very close to an AFM topological insulator that hosts robust edge states, can be well captured by a double-degenerate fragile topologically flat band just below the Fermi level. The Wilson loop calculations identify that such fragile topology is protected by the $S_{4z}$ symmetry, which gives rise to an AFM higher-order topological insulator that support the bound state with fractional charge $e/2$ at th…
The recent discovery of two-dimensional (2D) magnetic materials has brought magnetism to the flatland. This has opened up exciting opportunities for the exploration of fundamental physics as well as for novel device applications. Here, we predict a new thermodynamically stable 2D magnetic material, K$_2$CoS$_2$, which retains its in-plane anti-ferromagnetic order down to the monolayer and bilayer limits. We find that the magnetic moments ($2.5 μ_B/$Co) are aligned along the intra-Co chains, from monolayer to bulk. The non-magnetic electronic spectrum of both the monolayer and bilayer films is …
The topological states of matters arising from the nontrivial magnetic configuration provide a better understanding of physical properties and functionalities of solid materials. Such studies benefit from the active control of spin orientation in any solid, which is yet known to rarely take place in the two-dimensional (2D) limit. Here we demonstrate by the first-principles calculations that spin-orientation dependent topological states can appear in the geometrically frustrated monolayer antiferromagnet. Different topological states including quantum anomalous Hall (QAH) effect and time-rever…
Mermin-Wagner-Coleman theorem predicts no long-range magnetic order at finite temperature in the two-dimensional (2D) isotropic systems, but a quasi-long-range order with a divergent correlation length at the Kosterlitz-Thouless (KT) transition for planar magnets. As a representative of two-dimensional planar antiferromagnets, single-layer CoPS3 carries the promise of monolayer antiferromagnetic platforms for the ultimately thin spintronics. Here, with the aid of magnetostriction which is sensitive to the local magnetic order, we observe the signatured phonon mode splitting of below TKT in mon…
In this work, we studied the adsorption behavior of deposited Si atoms along with their diffusion and other dynamic processes on a Pb monolayer-covered Si(111) surface from 125-230 K using a variable-temperature scanning tunneling microscope (STM). The Pb-covered Si(111) surface form a low-symmetry row-like structure in this temperature range and the Si atoms bind favorably to two specific on-top sites (T1A and T1B) on the trimer row after deposition at the sample temperature of 125 K. The Si atoms were immobile at low temperatures and started to switch between the two neighboring T1A and T1B …
The novel properties of a uniaxially-expanded TiN bulk arising from increasing the layer spacing from equilibrium are explored using a first-principles approach. We reveal a novel nonmagnetic-magnetic transition from a TiN bulk to its monolayer. We also investigate the electronic and magnetic structures of a few TiN atomic layers. We find that the bilayer and trilayer, like the TiN bulk, are nonmagnetic poor metals. On the other hand, the monolayer TiN is found to carry a magnetic moment on its Ti atoms, and likely be a semiconductor. The unpaired electron giving rise to magnetism on Ti is pri…
We report the current-driven dynamics of frustrated skyrmions in an antiferromagnetically exchange coupled bilayer system, where the bilayer skyrmion consists of two monolayer skyrmions with opposite skyrmion numbers $Q$. We show that the in-plane current-driven bilayer skyrmion moves in a straight path, while the out-of-plane current-driven bilayer skyrmion moves in a circular path. It is found that the in-plane current-driven mobility of a bilayer skyrmion is much better than the monolayer one at a large ratio of $β/α$, where $α$ and $β$ denote the damping parameter and non-adiabatic spin tr…
A magnetic skyrmion is a topological magnetization structure with a nanometric size and a well-defined swirling spin distribution, which is anticipated to be an essential building block for novel skyrmion-based device applications. We study the motion of magnetic skyrmions in multilayer synthetic antiferromagnetic (SAF) racetracks as well as in conventional monolayer ferromagnetic (FM) racetracks at finite temperature. There is an odd-even effect of the constituent FM layer number on the skyrmion Hall effect (SkHE). Namely, due to the suppression of the SkHE, the magnetic skyrmion has no trans…
We present first-principles results on the structural, electronic, and magnetic properties of a new family of two-dimensional antiferromagnetic (AFM) manganese chalcogenides, namely monolayer MnX and Janus XMnY (X, Y= S, Se, Te), among which monolayer MnSe was recently synthesized in experiments [\href{https://pubs.acs.org/doi/abs/10.1021/acsnano.1c05532}{ACS Nano 15 (8),13794 (2021)}]. By carrying out calculations of the phonon dispersion and \textit{ab-initio} molecular dynamics simulations, we first confirmed that these systems, characterized by an unconventional strongly coupled bilayer at…
The van der Waals magnets CrX$_3$ (X = I, Br, and Cl) exhibit highly tunable magnetic properties and are promising candidates for developing novel two-dimensional (2D) magnetic devices such as magnetic tunnel junctions and spin tunneling transistors. Previous studies of CrCl$_3$ have mainly focused on mechanically exfoliated samples. Controlled synthesis of high quality atomically thin flakes is critical for their technological implementation but has not been achieved to date. Here, we report the growth of large CrCl$_3$ flakes with well-defined facets down to monolayer thickness (~0.6 nm) via…
Magnetism in two-dimensional materials is not only of fundamental scientific interest but also a promising candidate for numerous applications. However, studies so far, especially the experimental ones, have been mostly limited to the magnetism arising from defects, vacancies, edges or chemical dopants which are all extrinsic effects. Here, we report on the observation of intrinsic antiferromagnetic ordering in the two-dimensional limit. By monitoring the Raman peaks that arise from zone folding due to antiferromagnetic ordering at the transition temperature, we demonstrate that FePS3 exhibits…
We experimentally verify the existence of two model-type magnetic ground states which were previously predicted but so far unobserved. We find them in Mn monolayers on the Re(0001) surface using spin-polarized scanning tunneling microscopy. For fcc stacking of Mn the collinear row-wise antiferromagnetic state occurs, whereas for hcp Mn a three-dimensional spin structure appears, which is a superposition of three row-wise antiferromagnetic states and is known as triple-Q state. Density functional theory calculations elucidate the subtle interplay of different magnetic interactions to form these…
Optical signatures of antiferromagnetic correlations in a strongly interacting quantum Hall MoSe2 monolayer
Harvard University（哈佛大学）；Brookhaven National Laboratory（布鲁克海文国家实验室）；University of Connecticut（康涅狄格大学）；University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；Columbia University（哥伦比亚大学）；National Institute for Materials Science（国立材料研究所）
We investigate magnetic coupling between a monolayer of prototype single-molecule magnets Mn12 and a ferromagnetic Ni(111) substrate through S, using density-functional theory (DFT) and a DFT+U method. Our DFT and DFT+U calculations show that the Mn12 molecules favor antiferromagnetic coupling to the Ni substrate, and that they possess magnetic moments deviated from the magnetic moments of isolated Mn12 molecules. We find that the magnetic easy axis of the Mn12 on Ni (whole system) is dictated by that of the Ni substrate. The antiferromagnetic coupling is, dominantly, caused by superexchange i…
We propose a device concept, based on monolayer stanene, able to provide highly polarized spin currents (up to a $98\%$) with voltage-controlled spin polarization operating at room temperature and with small operating voltage ($0.3$ V). The concept exploits the presence of spin-polarized edge states in a stanene nanoribbon. The spin polarization of the total current can be modulated by a differential tuning of the transmission properties, and of the occupation of edge states of different spin, via the application of an in-plane electric field. We demonstrate device operation using ab-initio an…
It is essential to explore two-dimensional (2D) material with magnetic ordering in new generation spintronic devices. Particularly, the seeking of room-temperature 2D ferromagnetic (FM) materials is a hot topic of current research. Here, we study magnetism of the Mn-doped and electron-doped SiC monolayer using first-principle calculations. For the Mn-doped SiC monolayer, we find that either electron or hole could mediate the ferromagnetism in the system and the Curie temperature ($T_C$) can be improved by appropriate carrier doping. The codoping strategy is also discussed on improving $T_C$. T…
Lifting the valley degeneracy of monolayer transition metal dichalcogenides (TMD) would allow versatile control of the valley degree of freedom. We report a giant valley exciton splitting of 18 meV/T for monolayer WS2, using the proximity effect from a ferromagnetic EuS substrate, which is enhanced by nearly two orders of magnitude from the 0.2 meV/T obtained by an external magnetic field. More interestingly, a sign reversal of the valley exciton splitting is observed as compared to that of WSe2 on EuS. Using first principles calculations, we investigate the complex behavior of exchange intera…
Considerable research interest has been attracted to noncollinear magnetic structures for their intriguing physics and promising applications. In this work, based on relativistic density functional theory, we reveal the interesting magnetic order and relevant properties in monolayer RuF$_4$, which can be exfoliated from its bulk phase. Although the spins on Ru ions are almost antiferromagnetically aligned between nearest-neighbors, weak ferromagnetism is generated because of the antisymmetric Dzyaloshinskii-Moriya interaction as well as the single-ion anisotropy. A prominent magneto-optical Ke…
At high magnetic fields, monolayer graphene hosts competing phases distinguished by their breaking of the approximate SU(4) isospin symmetry. Recent experiments have observed an even denominator fractional quantum Hall state thought to be associated with a transition in the underlying isospin order from a spin-singlet charge density wave at low magnetic fields to an antiferromagnet at high magnetic fields, implying that a similar transition must occur at charge neutrality. However, this transition does not generate contrast in typical electrical transport or thermodynamic measurements and no d…
Spin waves in the bilayer van der Waals magnet CrSBr
Delft University of Technology（代尔夫特理工大学）；V.G. Baryakhtar Institute of Magnetism of the NAS of Ukraine（乌克兰国家科学院V.G.巴里亚赫塔尔磁学研究所）；Institute of Spintronics and Quantum Information, Faculty of Physics and Astronomy, Adam Mickiewicz University（亚当·密茨凯维奇大学物理与天文学学院自旋电子学与量子信息研究所）；WPI-AIMR & IMR & CSIS, Tohoku University（东北大学WPI-先进物质与器件研究所(IMR)及材料系统国际研究前沿中心(CSIS)）；Kavli Institute for Theoretical Sciences, University of the Chinese Academy of Sciences（中国科学院大学卡弗里理论科学研究所）
The recent discovery of magnetism in atomically thin layers of van der Waals (vdW) crystals has created new opportunities for exploring magnetic phenomena in the two-dimensional (2D) limit. In most 2D magnets studied to date the c-axis is an easy axis, so that at zero applied field the polarization of each layer is perpendicular to the plane. Here, we demonstrate that atomically thin CrCl3 is a layered antiferromagnetic insulator with an easy-plane normal to the c-axis, that is the polarization is in the plane of each layer and has no preferred direction within it. Ligand field photoluminescen…
We insert and manipulate a single chlorine atom in chlorine monolayer on a Si(100)-2x1 surface using a scanning tunneling microscope. Two objects were created - a Cl atom in a groove between two dimer rows, and bridge-bonded Cl on a silicon dimer. Changing the voltage polarity leads to conversion of the objects into each other. Anisotropic movement of the objects at 77 K is mediated by two different diffusion mechanisms: hopping and crowdion-like motion. Insertion of a Cl atom in a groove between two dimer rows leads to the formation of a dangling bond on a third-layer Si atom. At positive sam…
The recent discovery of two-dimensional (2D) magnetic materials which are compound of transition metal (TM) with other elements, has opened new avenues for basic research on low-dimensional magnetism and potential applications in spintronics. To further explore new 2D magnets of pure TM is thus of an interesting topic. Based on the first-principles calculations, here we propose a strategy of obtaining monolayer TM magnets, i.e., depositing TM atoms on graphyne (Gy) which has proper hexagonal hollow geometry. We find that TM monolayer with perfect hexagonal geometry can be formed on Gy. The TM …
The recently synthesized two-dimensional electride Gd$_2$C was proposed to be a ferromagnetic metal that possesses multiple pairs of Weyl points and may display a large anomalous Hall conductivity [Liu \textit{et al.}, Phys. Rev. Lett. \textbf{125}, 187203 (2020)]. In view of its layered structure, here we carry out first-principles studies on the magnetic and electronic properties of Gd$_2$C in the ultrathin monolayer limit. We find that monolayer Gd$_2$C remains ferromagnetic like the bulk form and the hydrogenation can effectively tune its magnetism and electronic structure. With one-sided …
We build a microscopic model to study the intra- and inter-layer superexchange due to electrons hopping in chromium trihalides ($\mathrm{CrX}_3$, X= Cl, Br, and I). In evaluating the superexchange, we identify the relevant intermediate excitations in the hopping. In our study, we find that the intermediate hole-pairs excitations in the $p$-orbitals on X ion play a crucial role in mediating various types of exchange interactions. In particular, the inter-layer antiferromagnetic exchange may be realized by the hole-pair-mediated superexchange. Interestingly, we also find that these virtual hoppi…
Intrinsic antiferromagnetism in van der Waals (vdW) monolayer (ML) crystals enriches the understanding regarding two-dimensional (2D) magnetic orders and holds special virtues over ferromagnetism in spintronic applications. However, the studies on intrinsic antiferromagnetism are sparse, owing to the lack of net magnetisation. In this study, by combining spin-polarised scanning tunnelling microscopy and first-principles calculations, we investigate the magnetism of vdW ML CrTe2, which has been successfully grown through molecular beam epitaxy. Surprisingly, we observe a stable antiferromagneti…
The integration of diverse electronic phenomena, such as magnetism and nontrivial topology, into a single system is normally studied either by seeking materials that contain both ingredients, or by layered growth of contrasting materials. The ability to simply stack very different two dimensional (2D) van der Waals materials in intimate contact permits a different approach. Here we use this approach to couple the helical edges states in a 2D topological insulator, monolayer WTe2, to a 2D layered antiferromagnet, CrI3. We find that the edge conductance is sensitive to the magnetization state of…
We propose a new type of spin-valley locking (SVL), named $\textit{C}$-paired SVL, in antiferromagnetic systems, which directly connects the spin/valley space with the real space, and hence enables both static and dynamical controls of spin and valley to realize a multifunctional antiferromagnetic material. The new emergent quantum degree of freedom in the $\textit{C}$-paired SVL is comprised of spin-polarized valleys related by a crystal symmetry instead of the time-reversal symmetry. Thus, both spin and valley can be accessed by simply breaking the corresponding crystal symmetry. Typically, …
Atomically thin chromium triiodide (CrI3) has recently been identified as a layered antiferromagnetic insulator, in which adjacent ferromagnetic monolayers are antiferromagnetically coupled. This unusual magnetic structure naturally comprises a series of anti-aligned spin filters which can be utilized to make spin-filter magnetic tunnel junctions with very large tunneling magnetoresistance (TMR). Here we report voltage control of TMR formed by four-layer CrI3 sandwiched by monolayer graphene contacts in a dual-gated structure. By varying the gate voltages at fixed magnetic field, the device ca…
We propose an atom-superposition-based method for simulating spin-polarized scanning tunneling microscopy (SP-STM) from first principles. Our approach provides bias dependent STM images in high spatial resolution, with the capability of using either constant current or constant height modes of STM. In addition, topographic and magnetic contributions can clearly be distinguished, which are directly comparable to results of SP-STM experiments in the differential magnetic mode. Advantages of the proposed method are that it is computationally cheap, it is easy to parallelize, and it can employ the…
A monolayer of CrI$_3$ is a two-dimensional crystal that in its equilibrium configuration is a ferromagnetic semiconductor, however, two coupled layers can be ferromagnetic or antiferromagnetic depending on the stacking. We study the magnetic phase diagram upon the strain of the antiferromagnetically coupled bilayer with C2/m symmetry. We found that strain may be an efficient tool to tune the magnetic phase of the structure. A tensile strain stabilizes the antiferromagnetic phase, while a compressive strain turns the system ferromagnetic. We understood that behavior by looking at the relative …
Conventional electronics are based invariably on the intrinsic degrees of freedom of an electron, namely, its charge and spin. The exploration of novel electronic degrees of freedom has important implications in both basic quantum physics and advanced information technology. Valley as a new electronic degree of freedom has received considerable attention in recent years. In this paper, we develop the theory of spin and valley physics of an antiferromagnetic honeycomb lattice. We show that by coupling the valley degree of freedom to antiferromagnetic order, there is an emergent electronic degre…
We study realizations of spirals and skyrmions in two-dimensional antiferromagnets with a triangular lattice on an inversion-symmetry-breaking substrate. As a possible material realization, we investigate the adsorption of transition-metal atoms (Cr, Mn, Fe, or Co) on a monolayer of MoS$_2$, WS$_2$, or WSe$_2$ and obtain the exchange, anisotropy, and Dzyaloshinskii-Moriya interaction parameters using first-principles calculations. Using energy minimization and parallel-tempering Monte-Carlo simulations, we determine the magnetic phase diagrams for a wide range of interaction parameters. We fin…
