Two-dimensional (2D) Janus semiconductors with mirror asymmetry can introduce novel properties, such as large spin-orbit coupling (SOC) and normal piezoelectric polarization, which have attracted a great interest for their potential applications. Inspired by the recently fabricated 2D ferromagnetic (FM) semiconductor CrI3, a stable 2D (in x-y plane) antiferromagnetic (AFM) Janus semiconductor Fe2Cl3I3 with normal sublattice magnetization (m//z) is obtained by density functional theory calculations. By applying a tensile strain, the four magnetic states sequentially occur: AFM with m//z of sublattice, AFM with m//xy of sublattice, FM with m//xy, and FM with m//z. Such novel magnetic phase diagram driven by strain can be well understood by the spin-spin interactions including the third nearest-neighbor hoppings with the single-ion anisotropy, in which the SOC of I atoms is found to play an essential role. In addition, the electric polarization of Fe2Cl3I3 preserves with strain due to the broken inversion symmetry. Our results predict the rare Janus material Fe2Cl3I3 as an example of 2D semiconductors with both spin and charge polarizations, and reveal the highly sensitive strain-controlled magnetic states and magnetization direction, which highlights the 2D magnetic Janus semiconductor as a new platform to design spintronic materials.
Antiferromagnetic skyrmion crystal (AF-SkX), a regular array of antiferromagnetic skyrmions, is a fundamental phenomenon in the field of condensed-matter physics. So far, only very few proposals have been made to realize the AF-SkX, and most based on three-dimensional (3D) materials. Herein, using first-principles calculations and Monte-Carlo simulations, we report the identification of AF-SkX in two-dimensional lattice of Janus monolayer CrSi2N2As2. Arising from the broken inversion symmetry and strong spin-orbit coupling, large Dzyaloshinskii-Moriya interaction is obtained in Janus monolayer…
Two-dimensional (2D) intrinsic ferromagnetic semiconductors are expected to stand out in the spintronic field. Recently, the monolayer VI$_{3}$ has been experimentally synthesized but the weak ferromagnetism and low Curie temperature ($T_C$) limit its potential application. Here we report that the Janus structure can elevate the $T_C$ to 240 K. And it is discussed that the reason for high $T_C$ in Janus structure originates from the lower virtual exchange gap between $t_{2g}$ and $e_{g}$ states of nearest-neighbor V atoms. Besides, $T_C$ can be further substantially enhanced by tensile strain …
Two-dimensional rare-earth Janus 2$\textit{H}$-Gd$\textit{XY}$ ($\textit{X}$,$\textit{Y}$=Cl, Br, I, $\textit{X}$$\neq$$\textit{Y}$) monolayers: Bipolar ferro-magnetic semiconductors with high Curie temperature and large valley polarization
Emergence of half-semiconductor behavior and tunable magnetism via carrier doping in Janus VXSe (X=Cl, Br, I) monolayers
Southwest University（西南大学）；Hanhong College, Southwest University（汉弘学院，西南大学）；AECC Hunan Aviation Powerplant Research Institute（中国航发湖南航空发动机研究所）；Chengdu University of Technology（成都理工大学）；Leshan Normal University（乐山师范学院）；Shanghai Jiao Tong University（上海交通大学）
Herein we demonstrate the ability to optically tune the mobility of electrically powered Janus particles (JP) that are half coated with various Zinc Oxide (ZnO) semiconducting layers, i.e. polycrystalline, amorphous and amorphous with a SiO2 passivation layer. The ZnO semiconductor photo-response enables increase in its electrical conductivity with light having wavelengths of sufficient photon energy with respect to the semiconductor bandgap. This effect, termed optically modulated electrokinetic propulsion (OMEP), can be harnessed to increase the contrast in polarizability between the dielect…
Inspired by the successful synthesis of two-dimensional (2D) V-based Janus dichloride monolayers with intrinsic ferromagnetism and high Curie temperature (T$_{c}$), the electronic structure, spin-valley splitting and magnetic anisotropy of Janus 2H-VSeS monolayers are investigated in detailed using first-principles calculations. The results show that the Janus 2H-VSeS monolayer exhibits a large valley splitting of 105meV, high T$_{c}$ of 278K and good magnetocrystalline anisotropy (0.31meV) contributed by the in-plane d$_{x^{2}-y^{2}}$/d$_{xy}$ orbitals of V atoms. The biaxial strain ($-$8%<$\…
Based on a rare-earth Gd atom with 4$f$ electrons, through first-principles calculations, we demonstrate that the Janus 2H-GdIBr monolayer exhibits an intrinsic ferromagnetic (FM) semiconductor character with an indirect band gap of 0.75 eV, high Curie temperature T$_{c}$ of 260 K, significant magnetic moment of 8 $μ_{B}$/f.u. (f.u.=formula unit), in-plane magnetic anisotropy (IMA) and large spontaneous valley polarization of 118 meV. The MAE, inter-atomic distance or angle, and T$_{c}$ can be efficiently modulated by in-plane strains and charge carrier doping. Under the strain range from $-$5…
We present first-principles results on the structural, electronic, and magnetic properties of a new family of two-dimensional antiferromagnetic (AFM) manganese chalcogenides, namely monolayer MnX and Janus XMnY (X, Y= S, Se, Te), among which monolayer MnSe was recently synthesized in experiments [\href{https://pubs.acs.org/doi/abs/10.1021/acsnano.1c05532}{ACS Nano 15 (8),13794 (2021)}]. By carrying out calculations of the phonon dispersion and \textit{ab-initio} molecular dynamics simulations, we first confirmed that these systems, characterized by an unconventional strongly coupled bilayer at…
Based on first-principles calculations, we studied the geometric configuration, stability and electronic structure of the two-dimensional Janus MoTeB2. The MoTeB2 monolayer is semimetal, and its attractive electronic structure reveals the perfect electron-hole compensation. Moreover, the electron-type and hole-type bands of the MoTeB2 monolayer are easily adjustable by external stain and charge doping, such as the switch of carrier polarity by charge doping, and the metal-semiconductor transition under tensile stain. These properties allow the MoTeB2 monolayer to be a controllable two-dimensio…
We study the electromechanical response of Janus transition metal dichalcogenide (TMD) nanotubes from first principles. In particular, considering both armchair and zigzag variants of twenty-seven select Janus TMD nanotubes, we determine the change in bandgap and charge carriers' effective mass upon axial and torsional deformations using density functional theory (DFT). We observe that metallic nanotubes remain unaffected, whereas the bandgap in semiconducting nanotubes decreases linearly and quadratically with axial and shear strains, respectively, leading to semiconductor--metal transitions.…
Two-dimensional (2D) niobium oxydihalide NbOI$_2$ has been recently demonstrated as an excellent in-plane piezoelectric and nonlinear optical materials. Here we show that Janus niobium oxydihalide, NbO$XY$ (X, Y = Cl, Br, I and X$\neq$Y), is a multifunctional anisotropic semiconductor family with exceptional piezoelectric, electronic, photocatalytic and optical properties. NbO$XY$ are stable and mechancially flexible monolayers with band gap around the visible light regime of $\sim 1.9$ eV. The anisotropic carrier mobility of NbO$XY$ lies in the range of $10^3 \sim 10^4$ cm$^2$V$^{-1}$s$^{-1}$…
The possibility of half-metallic antiferromagnetism, a special case of ferrimagnetism with a compensated magnetization, in the diluted magnetic semiconductors is highlighted on the basis of the first principles electronic structure calculation. As typical examples, the electrical and magnetic properties of II-VI compound semiconductors doped with 3d transition metal ion pairs--(V, Co) and (Fe, Cr)--are discussed.
Two-dimensional intrinsic antiferromagnetic semiconductors are expected to stand out in the spintronic field. The present work finds the monolayer T'-MoTeI is intrinsically an antiferromagnetic semiconductor by using first-principles calculation. Firstly, the dimerized distortion of the Mo atoms causes T'-MoTeI to have dynamic stability, which is different from the small imaginary frequency in the phonon spectrum of T-MoTeI. Secondly, T'-MoTeI is an indirect-bandgap semiconductor with 1.35 eV. Finally, in the systematic study of strain effects, there are significant changes in the electronic s…
Discovering new antiferromagnetic compounds is at the forefront of developing future spintronic devices without fringing magnetic fields. The antiferromagnetic gapless semiconducting D03 phase of V3Al was successfully synthesized via arc-melting and annealing. The antiferromagnetic properties were established through synchrotron measurements of the atom-specific magnetic moments, where the magnetic dichroism reveals large and oppositely-oriented moments on individual V atoms. Density functional theory calculations confirmed the stability of a type G antiferromagnetism involving only two-third …
Tuning topological and magnetic properties of materials by applying an electric field is widely used in spintronics. In this work, we find a topological phase transition from topologically trivial to nontrivial states at an external electric field of about 0.1 V/A in MnBi$_2$Te$_4$ monolayer that is a topologically trivial ferromagnetic semiconductor. It is shown that when electric field increases from 0 to 0.15 V/A, the magnetic anisotropy energy (MAE) increases from about 0.1 to 6.3 meV, and the Curie temperature Tc increases from 13 to about 61 K. The increased MAE mainly comes from the enh…
We study in this paper the parallel spin current in an antiferromagnetic semiconductor thin film where we take into account the interaction between itinerant spins and lattice spins. The spin model is an anisotropic Heisenberg model. We use here the Boltzmann's equation with numerical data on cluster distribution obtained by Monte Carlo simulations and cluster-construction algorithms. We study the cases of degenerate and non-degenerate semiconductors. The spin resistivity in both cases is shown to depend on the temperature with a broad maximum at the transition temperature of the lattice spin …
The electronic band structures of orthorhombic (oP28) and monoclinic (mC28) MnSb_2S_4 were investigated with ab initio calculations in the local spin density approximation (LSDA) to the density functional theory (DFT). An analysis of the electronic properties and of the chemical bonding is provided using the augmented spherical wave (ASW) method considering nonmagnetic, ferromagnetic, ferrimagnetic and antiferromagnetic model orderings. In agreement with experimental results both modifications of MnSb_2S_4 are predicted to be antiferromagnetic. While the experimental band gap is missed for the…
Emergence of Rashba splitting and spin-valley properties in Janus MoGeSiP2As2 and WGeSiP2As2 monolayers
International Research Centre MagTop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Department of Physics and Energy Harvest Storage Center, University of Ulsan（蔚山大学物理与能量收集中心）；College of Physics and Optoelectronic Engineering, Shenzhen University（深圳大学物理与光电工程学院）
Quantized spin-wave known as magnon, a bosonic quasiparticle, can drag electrons or holes via sd exchange interaction and boost the thermopower over the conventional diffusive thermopower. P-type magnon-drag thermopower has been observed in both ferromagnetic and antiferromagnetic metallic and degenerate semiconductors. However, it has been less reported for intrinsic or n-type magnetic semiconductors; therefore, the impact of magnon-bipolar carrier drag on thermopower has remained unexplored. Here, a theoretical model for magnon-bipolar carrier drag thermopower is derived based on the magnon-…
In this paper, the electrical and spin properties of mono- and bilayer HfSSe in the presence of a vertical electric field are studied. The density functional theory is used to investigate their properties. Fifteen different stacking orders of bilayer HfSSe are considered. The mono- and bilayer demonstrate an indirect bandgap, whereas the bandgap of bilayer can be effectively controlled by electric field. While the bandgap of bilayer closes at large electric fields and a semiconductor to metal transition occurs, the effect of a normal electric field on the bandgap of the monolayer HfSSe is quit…
After decades of research, the low Curie temperature of ferromagnetic semiconductors remains the key problem in the development of magnetic semiconductor spintronic technologies. Removing this roadblock might require a change of the field's basic materials paradigm by looking beyond ferromagnets. Recent studies of relativistic magnetic and magnetotransport anisotropy effects, which in principle are equally well present in materials with ferromagnetically and antiferromagnetically ordered spins, have inspired our search for antiferromagnetic semiconductors suitable for high-temperature spintron…
We use sensitive dynamic cantilever magnetometry to measure the magnetic hysteresis of individual magnetic Janus particles. These particles consist of hemispherical caps of magnetic material deposited on micrometer-scale silica spheres. The measurements, combined with corresponding micromagnetic simulations, reveal the magnetic configurations present in these individual curved magnets. In remanence, ferromagnetic Janus particles are found to host a global vortex state with vanishing magnetic moment. In contrast, a remanent onion state with significant moment is recovered by imposing an exchang…
Searching for novel antiferromagnetic materials with large magnetotransport response is highly demanded for constructing future spintronic devices with high stability, fast switching speed, and high density. Here we report a colossal anisotropic magnetoresistance effect in an antiferromagnetic binary compound with layered structure rare-earth dichalcogenide EuTe2. The AMR reaches 40000%, which is 4 orders of magnitude larger than that in conventional antiferromagnetic alloys. Combined magnetization, resistivity, and theoretical analysis reveal that the colossal AMR effect is attributed to a no…
The already intriguing electronic and optical properties of the MXene Sc2C family can be further tuned through a wide range of possible functionalizations. Here, by means of Density Functional Theory, we show that the 36 possible elements of the Janus MXT (M:Sc2C, X:O, F, OH, T:C, N, S) family, built by considering the four possible structural models (i) FCC, (ii) HCP , (iii) FCC + HCP, and (iv) HCP + FCC, are all potentially stable. The analysis of their mechanical properties shows the excellent mechanical flexibility of functionalized MXenes (f-MXenes) under large strain, making them more su…
In this computational work based on density functional theory we study the electronic and electron transport properties of asymmetric multi-layer MoSSe junctions, known as Janus junctions. Focusing on 4-layer systems, we investigate the influence of electric field, electrostatic doping, strain, and interlayer stacking on the electronic structure. We discover that a metal to semiconductor transition can be induced by an out-of-plane electric field. The critical electric field for such a transition can be reduced by in-plane biaxial compressive strain. Due to an intrinsic electric field, a 4-lay…
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…
The seminal experimental discovery of the remarkably stable MoSi$_2$N$_4$ monolayer has led to a handful of predicted magnetic two-dimensional (2D) materials in the MA$_2$Z$_4$ family (M = transition metals, A = Si, Ge, and Z = N, P, As). These magnetic monolayers were predicted to be dynamically stable, but none of them has been synthesized to date. In this Research Letter, from first-principles thermodynamic stability analysis, we demonstrate that only the nitrides are thermodynamically stable and this occurs under N-rich conditions. Based on this finding, we propose two ferromagnetic, semic…
In analogy to transition-metal dichalcogenide (TMD) monolayers, which have wide applications in photoelectricity, piezoelectricity and thermoelectricity, Janus MoSSe monolayer has been successfully synthesized by substituting the top Se atomic layer in $\mathrm{MoSe_2}$ by S atoms. In this work, Janus monolayer ZrSSe is proposed by ab initio calculations. For the electron part, the generalized gradient approximation (GGA) plus spin-orbit coupling (SOC) is used as exchange-correlation potential, while GGA for lattice part. Calculated results show that the ZrSSe monolayer is dynamically and mech…
Structure-property relationships have always been guiding principles in discovering new materials. Here we explore the relationships to discover novel two-dimensional (2D) materials with the goal of identifying 2D magnetic semiconductors for spintronics applications. In particular, we report a density functional theory + $U$ study of single-layer antiferromagnetic (AFM) semiconductor CoS$_2$ with the pentagonal structure forming the so-called Cairo Tessellation. We find that this single-layer magnet exhibits an indirect bandgap of 1.06 eV with light electron and hole effective masses of 0.03 a…
Janus two-dimensional (2D) materials have attracted much attention due to possessing unique properties caused by their out-of-plane asymmetry, which have been achieved in many 2D families. In this work, the Janus monolayers are predicted in new 2D $\mathrm{MA_2Z_4}$ family by means of first-principles calculations, $\mathrm{MoSi_2N_4}$ and $\mathrm{WSi_2N_4}$ of which have been synthesized in experiment(\textcolor[rgb]{0.00,0.00,1.00}{Science 369, 670-674 (2020)}). The predicted $\mathrm{MSiGeN_4}$ (M=Mo and W) monolayers exhibit dynamic, thermodynamical and mechanical stability, and they are …
Converting solar energy into chemical energy by splitting water is a promising means to generate a sustainable and renewable solution without detrimental environmental impact. The two-dimensional semiconductors serve as potential catalysts in this regard, and here we combine Janus transition-metal dichalcogenides (MoXY, X/Y = S, Se, Te) and graphitic carbon nitride in a van der Waals heterostructure. Within the first-principles calculations, we investigate the electronic, optical and excitonic properties that determine the photocatalytic activity. Due to the internal electric field, the photog…
It has been proposed that antiferromagnetic Fe adatom spins on semiconductor Cu-N surfaces can be used to store information [S. Loth {\it et al}, Science \textbf{335}, 196 (2012)]. Here, we investigate spin dynamics of such antiferromagnetic systems through Monte Carlo simulations. We find out the temperature and size laws of switching rates of Néel states and show that the Néel states can become stable enough for the information storage when the number of spins reaches to one or two dozens of the Fe spins. We also explore promising methods for manipulating the Néel states. These could help re…
We report electrical and thermal transport properties of Mn-based material BaMn$_2$Bi$_2$ with ThCr$_2$Si$_2$ structure. The resistivity of the antiferromagnetic BaMn$_2$Bi$_2$ shows a metal-semiconductor transition at $\sim 80$ K with decreasing temperature. Correspondingly, the thermopower $S$ shows a peak at the same temperature, approaching ~150 $μ$V/K. With increasing temperature $S$ decreases to about 125 $μ$V/K at the room temperature. The magnetic field enhances the peak value to 210 $μ$V/K. The Hall resistivity reveals an abrupt change of the carrier density close to the metal-semicon…
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 contribution of bulk and surface to the electrical resistance along crystallographic \textit{b}- and \textit{c}-axes as a function of crystal thickness gives evidence for a temperature independent surface states in an antiferromagnetic narrow-gap semiconductor CrSb$_{2}$. ARPES shows a clear electron-like pocket at $Γ$-$Z$ direction which is absent in the bulk band structure. First-principles calculations also confirm the existence of metallic surface states inside the bulk gap. Whereas combined experimental probes point to enhanced surface conduction similar to topological insulators, sur…
