Topological spin structures, such as magnetic skyrmions, hold great promises for data storage applications, thanks to their inherent stability. In most cases, skyrmions are stabilized by magnetic fields in non-centrosymmetric systems displaying the chiral Dzyaloshinskii-Moriya exchange interaction, while spontaneous skyrmion lattices have been reported in centrosymmetric itinerant magnets with long-range interactions. Here, a spontaneous anti-biskyrmion lattice with unique topology and chirality is predicted in the monolayer of a semiconducting and centrosymmetric metal halide, NiI$_2$. Our first-principles and Monte Carlo simulations reveal that the anisotropies of the short-range symmetric exchange, when combined with magnetic frustration, can lead to an emergent chiral interaction that is responsible for the predicted topological spin structures. The proposed mechanism finds a prototypical manifestation in two-dimensional magnets, thus broadening the class of materials that can host spontaneous skyrmionic states.
Quantum Spin Hall (QSH) insulators with a large topologically nontrivial bulk gap are crucial for future applications of the QSH effect. Among these, group III-V monolayers and their halides with chair structure (regular hexagonal framework, RHF) were widely studied. Using first-principles calculations, we propose a new structure model for the functionalized group III-V monolayers, which consist of rectangular GaBi-X2 (X=I, Br, Cl) monolayers with a distorted hexagonal framework (DHF). These structures have a much lower energy than the GaBi-X2 monolayers with chair structure. Remarkably, the D…
Two-dimensional (2D) magnets have great potentials for applications in next-generation information devices. Since the recent experimental discovery of intrinsic 2D magnetism in monolayer CrI$_3$ and few-layer Cr$_2$Ge$_2$Te$_6$, intensive studies have been stimulated in pursuing more 2D magnets and revealing their intriguing physical properties. In comparison to the magnetism based on $3d$ electrons, $4f$ electrons can provide larger magnetic moments and stronger spin-orbit coupling, but have been much less studied in the 2D forms. Only in very recent years, some exciting results have been obt…
Magnetic skyrmions are nano-scale spin structures that are promising for ultra-dense memory and logic devices. Recent progresses in two-dimensional magnets encourage the idea to realize skyrmionic states in freestanding monolayers. However, monolayers such as CrI3 lack Dzyaloshinskii-Moriya interactions (DMI) and thus do not naturally exhibit skyrmions but rather a ferromagnetic state. Here we propose the fabrication of Cr(I,X)3 Janus monolayers, in which the Cr atoms are covalently bonded to the underlying I ions and top-layer Br or Cl atoms. By performing first-principles calculations and Mo…
The realization of multiferroics in nanostructures, combined with a large electric dipole and ferromagnetic ordering, could lead to new applications, such as high-density multi-state data storage. Although multiferroics have been broadly studied for decades, ferromagnetic ferroelectricity is rarely explored, especially in two-dimensional (2D) systems. Here we report the discovery of 2D ferromagnetic ferroelectricity in layered transition metal halide systems. On the basis of first-principles calculations, we reveal that charged CrBr3 monolayer exhibits in-plane multiferroicity, which is ensure…
Chemical vapor deposition (CVD) of two-dimensional (2D) tungsten dichalcogenide crystals requires steady flow of tungsten source in the vapor phase. This often requires high temperature and low pressure due to the high sublimation point of tungsten oxide precursors. We demonstrate atmospheric pressure CVD of WSe2 and WS2 monolayers at moderate temperatures (700 ~ 850 oC) using alkali metal halides (MX where M= Na or K and X=Cl, Br or I) as the growth promoters. We attribute the facilitated growth to the formation of volatile tungsten oxyhalide species during growth, which leads to efficient de…
Quantum spin Hall (QSH) insulators possess edge states that are topologically protected from backscattering. However, known QSH materials (e.g. HgTe/CdTe and InAs/GaSb quantum wells) exhibit very small energy gap and only work at low temperature, hindering their applications for room temperature devices. Based on the first-principles calculations, we predict a novel family of QSH insulators in monolayer tantalum carbide halide TaCX (X = Cl, Br, and I) with unique rectangular lattice and large direct energy gaps larger than 0.2 eV, accurately, 0.23$-$0.36 eV. The mechanism for 2D QSH effect in …
The intrinsic magnetism observed in two-dimensional (2D) van der Waals (vdW) materials provides a unique opportunity for exploring the 2D topological magnetic textures, in particular skyrmionic magnetic textures (SMTs) including skyrmion and its topological equivalents. Since the experimental discovery of skyrmions in the 2D vdW materials and their heterostructures, a critical challenge lies in the control of these SMTs to translate their intriguing features into spintronic applications. Here, we review the recent experimental and theoretical progresses on the modulations of SMTs in 2D vdW mon…
Two-dimensional multiferroic materials are highly sought after due to their huge potential for applications in nanoelectronic and spintronic devices. Here, we predict, based on first-principle calculations, a single phase {\it triferroic} where three ferroic orders; ferromagnetism, ferroelectricity and ferroelasticity, coexist simultaneously in hole doped GdCl$_2$ monolayer (a ferromagnetic semiconductor). This is achieved by substituting 1/3rd of the Gd$^{2+}$ ions with Eu$^{2+}$ in the hexagonal structure of GdCl$_2$ monolayer. The resulting metallic state undergoes a bond-centered charge or…
Theoretical and experimental studies present that metal halogens in MX$_3$ forms can show very interesting electronic and magnetic properties in their bulk and monolayer phases. Many MX$_3$ materials have layered structures in their bulk phases, while RuBr$_3$ and RuI$_3$ have one-dimensional chains in plane. In this paper, we show that these metal halogens can also form two-dimensional layered structures in the bulk phase similar to other metal halogens, and cleavage energy values confirm that the monolayers of RuX$_3$ can be possible to be synthesised. We also find that monolayers of RuX$_3$…
Organohalide perovskite with a variety of surface structures and morphologies have shown promising potential owing to the choice of the type of heterostructure dependent stability. We systematically investigate and discuss the impact of 2-dimensional molybdenum-disulphide (MoS2), molybdenum-diselenide (MoSe2), tungsten-disulphide (WS2), tungsten-diselenide (WSe2), boron- nitiride (BN) and graphene monolayers on band-gap and energy stability of organic-inorganic halide perovskites. We found that MAPbI3ML deposited on BN-ML shows room temperature stability (-25 meV~300K) with an optimal bandgap …
Using first-principles calculations, we investigate six transition-metal nitride halides (TMNHs): HfNBr, HfNCl, TiNBr, TiNCl, ZrNBr, and ZrNCl as potential van der Waals (vdW) dielectrics for transition metal dichalcogenide (TMD) channel transistors. We calculate the exfoliation energies and bulk phonon energies and find that the six TMNHs are exfoliable and thermodynamically stable. We calculate both the optical and static dielectric constants in the in-plane and out-of-plane directions for both monolayer and bulk TMNHs. In monolayers, the out-of-plane static dielectric constant ranges from 5…
Using the tight-binding method in combination with first-principles calculations, we systematically derive a low-energy effective Hilbert subspace and Hamiltonian with spin-orbit coupling for two-dimensional hydrogenated and halogenated group-V monolayers. These materials are proposed to be giant-gap quantum spin Hall insulators with record huge bulk band gaps opened by the spin-orbit coupling at the Dirac points, e.g., from 0.74 to 1.08 eV in Bi\textit{X} (\textit{X} = H, F, Cl, and Br) monolayers. We find that the low-energy Hilbert subspace mainly consists of $p_{x}$ and $p_{y}$ orbitals fr…
Two dimensional magnetic materials, with tunable electronic properties could lead to new spintronic, magnetic and magneto-optic applications. Here, we explore intrinsic magnetic ordering in two dimensional monolayers of transition metal tri-halides (MX$_3$, M = V, Cr, Mn, Fe and Ni, and X = F, Cl, Br and I), using density functional theory. We find that other than FeX$_3$ family which has an anti-ferromagnetic ground state, rest of the trihalides are ferromagnetic. Amongst these the VX$_3$ and NiX$_3$ family are found to have the highest magnetic transition temperature, beyond the room tempera…
Valley- and Spin-Dependent Electronic and Transport Properties of Two-Dimensional Altermagnetic Titanium-Based Chalcogenide Halides
Northwest University（西北大学）；Shaanxi Key Laboratory for Theoretical Physics Frontiers（陕西省理论物理前沿重点实验室）；Peng Huanwu Center for Fundamental Theory（彭桓武基础理论研究中心）；Fundamental Discipline Research Center for Quantum Science and Technology of Shaanxi Province（陕西省量子科学与技术基础学科研究中心）
The chiral spin textures of a two-dimensional (2D) triangular system, where both antiferromagnetic (AF) Heisenberg exchange and chiral Dzyaloshinsky-Moriya interactions co-exist, are investigated numerically with an optimized quantum Monte Carlo method based on mean-field theory. We find that: helical, skyrmionic and vortical AF crystals can be formed when an external magnetic field is applied perpendicular to the 2D monolayer; the sizes of these skyrmions and vortices change abruptly at several critical points of the external magnetic field; each of these AF crystals can be decomposed into th…
Topological insulators (TIs) are promising for achieving dissipationless transport devices due to the robust gapless states inside the insulating bulk gap. However, currently realized 2D TIs, quantum spin Hall (QSH) insulators, suffer from ultra-high vacuum and extremely low temperature. Thus, seeking for desirable QSH insulators with high feasibility of experimental preparation and large nontrivial gap is of great importance for wide applications in spintronics. Based on the first-principles calculations, we predict a novel family of two-dimensional (2D) QSH insulators in transition-metal hal…
Design of 2D Skyrmionic Metamaterial Through Controlled Assembly
Uppsala University（乌普萨拉大学）；KTH Royal Institute of Technology（瑞典皇家理工学院）；Swedish e-Science Research Center（瑞典电子科学研究中心）；Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences（中国科学院深圳先进技术研究院）；Linnaeus University（林奈大学）；Örebro University（厄勒布鲁大学）；Soochow University（苏州大学）
Chromium iodide monolayers, which have different magnetic properties in comparison to the bulk chromium iodide, have been shown to form skyrmionic states in applied electromagnetic fields or in Janus-layer devices. In this work, we demonstrate that spin-canted solutions can be induced into monolayer chromium iodide by select substitution of iodide atoms with isovalent impurities. Several concentrations and spatial configurations of halide substitutional defects are selected to probe the coupling between the local defect-induced geometric distortions and orientation of chromium magnetic moments…
In order to search for states specific to insulator/metal interfaces, we have studied epitaxially grown interfaces with element-selective near edge X-ray absorption fine structure (NEXAFS). An extra peak is observed below the bulk edge onset for LiCl films on Cu and Ag substrates. The nature of chemical bonds as probed by X-ray photoemission spectroscopy and Auger electron spectroscopy remains unchanged, so we regard this as evidence for metal-induced gap states(MIGS) formed by the proximity to a metal, rather than local bonds at the interface. The dependence on the film thickness shows that t…
Hybrid lead halide perovskites with 2D stacking structures have recently emerged as promising materials for optoelectronic applications. We report a method for growing 2D nanosheets of hybrid lead halide perovskites (I, Br and Cl), with tunable lateral sizes ranging from 0.05 to 8 microns, and a structure consisting of n stacked monolayers separated by long alkylamines, tunable from bulk down to n=1. The key to obtaining such a wide range of perovskite properties hinged on utilizing the respective lead halide nanosheets as precursors in a hot-injection synthesis that afforded careful control o…
Chiral spin textures are fundamentally interesting, with promise for device applications. Stabilizing chirality is conventionally achieved by introducing Dzyaloshinskii-Moriya interaction (DMI) in asymmetric multilayers where the thickness of each layer is at least a few monolayers. Here we report an ultrasensitive chirality switching in (Ni/Co)n multilayer induced by capping with only 0.22 monolayer of Pd. Using spin-polarized low-energy electron microscopy, we monitor the gradual evolution of domain walls from left-handed to right-handed Neel walls and quantify the DMI induced by the Pd capp…
Two-dimensional van der Waals Janus materials and their heterostructures offer fertile platforms for designing fascinating functionalities. Here, by means of systematic first-principles studies on van der Waals Janus monolayer Cr-based dichalcogenide halides CrYX (Y=S, Se, Te; X=Cl, Br, I), we find that CrSX (X=Cl, Br, I) are the very desirable high TC ferromagnetic semiconductors with an out-of-plane magnetization. Excitingly, by the benefit of the large magnetic moments on ligand S2- anions, the sought-after large-gap quantum anomalous Hall effect and sizable valley splitting can be achieved…
Two-dimensional (2D) metal halides have received more attention because of their electronic and optoelectronic properties. Recently, researchers are interested to investigate the thermoelectric properties of metal halide monolayers because of their ultralow lattice conductivity, high Seebeck coefficient and figure of merit. Here, we have investigated thermoelectric and optoelectronic properties of XI$_2$ (X=Sn and Si) monolayers with the help of density functional theory and Boltzmann transport equation. The structural parameters have been optimized with relaxation of atomic positions. Excelle…
Exciton-polaritons offer a versatile platform for realization of all-optical integrated logic gates due to the strong effective optical nonlinearity resulting from the exciton-exciton interactions. In most of the current excitonic materials there exists a direct connection between the exciton robustness to thermal fluctuations and the strength of exciton-exciton interaction, making materials with highest levels of exciton nonlinearity applicable at cryogenic temperatures only. Here, we show that strong polaronic effects, characteristic for perovskite materials, allow to overcome this limitatio…
The magnetic properties of materials based on two-dimensional transition-metal dichalcogenides (TMDC) have been investigated by means of first-principles DFT calculations, namely Fe-intercalated bulk Fe$_{1/4}$TaS$_2$ compounds as well as TMDC monolayers with deposited Fe films. Changing the structure and the composition of systems consisting of Fe overlayers on top of a TMDC monolayers resulted in considerable variations of their physical properties. For the considered systems the Dzyaloshinskii-Moriya (DM) interaction has been determined and used for the subsequent investigation of their mag…
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…
Monolayer chromium trihalides, the archetypal two dimensional (2D) magnetic materials, are readily suggested as a promising platform for high frequency magnonics. Here we detail the spin wave properties of monolayer CrBr$_3$ and CrI$_3$, using spin dynamics simulations parametrized from the first principles. We reveal that spin wave dispersion can be tuned in a broad range of frequencies by strain, paving the way towards flexo magnonic applications. We further show that ever present halide vacancies in these monolayers host sufficiently strong Dzyaloshinskii Moriya interaction to scatter spin …
Dzyaloshinskii-Moriya interaction (DMI) is the primary mechanism for realizing real-space chiral spin textures, which are regarded as key components for the next-generation spintronics. However, DMI arises from a perturbation term of the spin-orbit interaction and is usually weak in pristine magnetic semiconductors. To date, large DMI and the resulting skyrmions are only realized in a few materials under stringent conditions. Using first-principles calculations, we demonstrate that significant DMI occurs between nearest-neighbor Cr atoms in two-dimensional (2D) magnetic semiconductor CrI$_3$ o…
It has been predicted theoretically and indirectly confirmed experimentally that single-layer CrX$_3$ (X=Cl, Br, I) might be the prototypes of topological magnetic insulators (TMI). In this work, by using first-principles calculations combined with atomistic spin dynamics we provide a complete picture of the magnetic interactions and magnetic excitations in CrX$_3$. The focus is here on the two most important aspects for the actual realization of TMI, namely the relativistic magnetic interactions and the finite-size (edge) effects. We compute the full interaction tensor, which includes both Ki…
Spin $\frac{1}{2}$ honeycomb materials have gained substantial interest due to their exotic magnetism and possible application in quantum computing. However, in all current materials out-of-plane interactions are interfering with the in-plane order, hence a true 2D magnetic honeycomb system is still of demand. Here, we report the exfoliation of the magnetic semiconductor $α$-RuCl$_3$ into the first halide monolayers and the magnetic characterization of the spin $\frac{1}{2}$ honeycomb arrangement of turbostratically stacked RuCl$_3$ monolayers. The exfoliation is based on a reductive lithiatio…
Complex magnetic exchange, anisotropy and skyrmionic textures in two-dimensional FeXZ$_{2}$ (\textit{X} = Nb, Ta and \textit{Z} = S, Se, Te) ferromagnets
Van der Waals (vdW) solids, as a new type of artificial materials that consist of alternating layers bonded by weak interactions, have shed light on fascinating optoelectronic device concepts. As a result, a large variety of vdW devices have been engineered via layer-by-layer stacking of two-dimensional materials, although shadowed by the difficulties of fabrication. Alternatively, direct growth of vdW solids has proven as a scalable and swift way, highlighted by the successful synthesis of graphene/h-BN and transition metal dichalcogenides (TMDs) vertical heterostructures from controlled vapo…
The moiré engineering of two-dimensional magnets opens unprecedented opportunities to design novel magnetic states with promises for spintronic device applications. The possibility of stabilizing skyrmions in these materials without chiral spin-orbit couplings or dipolar interactions is yet to be explored. Here, we investigate the formation and control of ground state topological spin textures (TSTs) in moiré CrI3 using stochastic Landau-Lifshitz-Gilbert simulations. We unveil the emergence of interlayer vortex and antivortex Heisenberg exchange fields, stabilizing spontaneous and field-assist…
