In flat-band materials, the strong Coulomb interaction between electrons can lead to exotic physical phenomena. Recently, $α$-In$_2$Se$_3$ thin films were found to possess ferroelectricity and flat bands. In this work, using first-principles calculations, we find that for the monolayer, there is a Weyl point at $Γ$ in the flat band, where the inclusion of the spin-orbit coupling opens a gap. Shifting the Fermi level into the spin-orbit gap gives rise to nontrivial band topology, which is preserved for the bilayer regardless of the interlayer polarization couplings. We further calculate the Chern number and edge states for both the monolayer and bilayer, for which the results suggest that they become quantum anomalous Hall insulators under appropriate dopings. Moreover, we find that the doping-induced magnetism for In$_2$Se$_3$ bilayer is strongly dependent on the interlayer polarization coupling. Therefore, doping the flat bands in In$_2$Se$_3$ bilayer can also yield multiferroicity, where the magnetism is electrically tunable as the system transforms between different polarization states. Our study thus reveals that multiferroicity and nontrivial band topology can be unified into one material for designing multifunctional electronic devices.
Polycrystalline YMn1-xFexO3 (YMFO_x) (0 <= x <= 0.1) compounds have been prepared in single phase and characterized by synchrotron X-ray diffraction, X-ray absorption near edge spectroscopy, magnetization, and dielectric measurements. Iron-substitution in hexagonal YMnO3 causes intra-lattice changes exceeding those of the lattice cell. XANES provide mixed-valence Mn3+/Mn4+ and Fe4+ charge states in these manganites, consistent with the observed decrease of the effective magnetic moment with Fe-doping. Magnetization M(T) evidence antiferromagnetic (AFM) ordering of the specimens with little wea…
The Haldane spin-chain compound, Tb2BaNiO5, with two antiferromagnetic transitions, one at T1=63K, and the other at T2=25K, has been recently shown by us to be an exotic multiferroic below T2. Here, we report the results of our investigations of Sr doping at the Ba site by magnetization, heat-capacity, magnetoelectric (MDE), and pyrocurrent measurements. An intriguing finding, which we stress, is that the ferroelectricity is lost even for a doping level of 10 atomic percent, though magnetic ordering prevails. The doped specimens however retain significant magnetodielectric behaviour, but with …
Ferromagnetism and orbital order in a topological ferroelectric
我们探索通过密度泛函计算的磁性掺杂的拓扑铁电体作为一种非常规的路线，多铁性。层状钙钛矿La $_{2}$ Ti $_{2}$ O $_{7}$的钒掺杂在很大程度上保持了电极化的强度并产生了稳健的铁磁有序性，因此具有适当的多铁性。掺杂剂聚集成链的显著趋势导致在一般掺杂下的绝缘特性。铁磁性源于多轨道V系统通过不寻常的“反铁”轨道顺序的对称性破缺，以及宿主的低对称性层状结构。
The orthorhombic Haldane spin chain compound Tb2BaNiO5 (Neel order, TN1= 63 K) has been shown to be an exotic multiferroic system below (TN2) 25 K due to various fascinating features, pointing to a strong potential for the advancement of concepts in this field. In particular, the rare-earth ions play a direct decisive role unlike in many other well known multiferroic materials and there appears to be a critical canting angle, developing below TN2, subtended by Tb 4f and Ni 3d moments to trigger this cross coupling phenomenon. However, for a small replacement of Sr for Ba, viz. in Tb2Ba0.9Sr0.1…
Fe doping into BaTiO3, stabilizes the paraelectric hexagonal phase in place of the ferroelectric tetragonal one [P. Pal et al. Phys. Rev. B, 101, 064409 (2020)]. We show that simultaneous doping of Bi along with Fe into BaTiO3 effectively enhances the magnetoelectric (ME) multiferroic response (both ferromagnetism and ferroelectricity) at room-temperature, through careful tuning of Fe valency along with the controlled-recovery of ferroelectric-tetragonal phase. We also report systematic increase in large dielectric constant values as well as reduction in loss tangent values with relatively mod…
The realization of multiferroicity in 2D nanomaterials is crucially important for designing advanced nanoelectronic devices such as non-volatile multistate data storage. In this work, the coexistence of ferromagnetism and ferroelectricity is reported in monolayer SnTe system by transition metal (TM) doping. Based on first-principles calculations, the spontaneous spin polarization could be realized by TM doping in ferroelectric SnTe monolayer. In addition to in-plane ferroelectric polarization, the out-of-plane ferroelectric polarization emerges in Mn (Fe)-doped SnTe monolayer due to the intern…
One of the most exciting properties of two dimensional materials is their sensitivity to external tuning of the electronic properties, for example via electric field or strain. Recently discovered analogues of phosphorene, group-IV monochalcogenides (MX with M = Ge, Sn and X = S, Se, Te), display several interesting phenomena intimately related to the in-plane strain, such as giant piezoelectricity and multiferroicity, which combine ferroelastic and ferroelectric properties. Here, using calculations from first principles, we reveal for the first time giant intrinsic spin Hall conductivities (S…
A key challenge in manipulating the magnetization in heavy-metal/ferromagnetic bilayers via the spin-orbit torque is to identify materials that exhibit an efficient charge-to-spin current conversion. Ab initio electronic structure calculations reveal that the intrinsic spin Hall conductivity (SHC) for pristine $β$-W is about sixty percent larger than that of $α$-W. More importantly, we demonstrate that the SHC of $β$-W can be enhanced via Ta alloying. This is corroborated by spin Berry curvature calculations of W$_{1-x}$Ta$_x$ ($x$ $\sim$ 12.5%) alloys which show a giant enhancement of spin Ha…
Bi$_{2}$Se$_{3}$, one of the most widely studied topological insulators (TIs), is naturally electron-doped due to n-type native defects. However, many years of efforts to achieve p-type Bi$_{2}$Se$_{3}$ thin films have failed so far. Here, we provide a solution to this long-standing problem, showing that the main culprit has been the high density of interfacial defects. By suppressing these defects through an interfacial engineering scheme, we have successfully implemented p-type Bi$_{2}$Se$_{3}$ thin films down to the thinnest topological regime. On this platform, we present the first tunable…
The realization of the Quantum anomalous Hall effect (QAHE) in two dimensional (2D) metal organic frameworks (MOFs), (MC$_4$S$_4$)$_3$ with M = Mn, Fe, Co, Ru and Rh, has been investigated based on a combination of first-principles calculations and tight binding models. Our results for the magnetic anisotropy energy (MAE) reveal that the out-of-plane (in-plane) magnetization is favored for M = Mn, Fe, and Ru (Co, and Rh). Given the structural symmetry of (MC$_4$S$_4$)$_3$, the QAHE takes place only for M = Mn, Fe and Ru. Such a quantum anomalous Hall phase has been confirmed through the calcul…
We investigate how field-effect doping affects the structural properties, the electronic structure and the Hall coefficient of few-layers transition metal dichalcogenides by using density-functional theory. We consider mono-, bi-, and trilayers of the H polytype of MoS2, MoSe2, MoTe2, WS2, and WSe2 and provide a full database of electronic structures and Hall coefficients for hole and electron doping. We find that, for both electron and hole doping, the electronic structure depends on the number of layers and cannot be described by a rigid band shift. Furthermore, it is important to relax the …
Anomalous Hall enhancement in fully compensated non-collinear antiferromagnetic Cr-doped Mn3Sn
National University of Singapore（新加坡国立大学）；National University of Singapore (Chongqing) Research Institute（新加坡国立大学（重庆）研究院）；Nanyang Technological University（南洋理工大学）；Nanjing University（南京大学）；Central South University（中南大学）
We report the critical role of La doping in the topological Hall effect observed in LaxEu1-xO thin films (~ 50 nm) grown by molecular beam epitaxy. When the La doping exceeds 0.036, topological Hall effect emerges, which we attribute to the formation of magnetic skyrmions. Besides, the La doping is found to play a critical role in determining the phases, densities, and sizes of the skyrmions in the LaxEu1-xO thin films. The maximum region of the skyrmion phase diagram is observed on the La0.1Eu0.9O thin film. As the La doping increases, the skyrmion density increases while the skyrmion size de…
Symmetry often governs condensed matter physics. The act of breaking symmetry spontaneously leads to phase transitions, and various observables or observable physical phenomena can be directly associated with broken symmetries. Examples include ferroelectric polarization, ferromagnetic magnetization, optical activities (including Faraday and magneto-optic Kerr rotations), second harmonic generation, photogalvanic effects, nonreciprocity, various Hall-effect-type transport properties, and multiferroicity. Herein, we propose that observable physical phenomena can occur when specimen constituents…
The interlayer antiferromagnetic coupling hinders the observation of quantum anomalous Hall effect in magnetic topological insulator MnBi$_2$Te$_4$. We demonstrate that interlayer \textit{ferromagnetism} can be established by utilizing the \textit{p}-doping method in MnBi$_2$Te$_4$ multilayers. In two septuple-layers system, the interlayer ferromagnetic coupling appears by doping nonmagnetic elements (e.g., N, P, As, Na, Mg, K, and Ca), due to the redistribution of orbital occupations of Mn. We further find that Mg and Ca elements are the most suitable candidates because of their low formation…
Topological materials are expected to show distinct transport signatures due to their unique band-inversion character and band-crossing points. However, the intentional modulation of such topological responses by experimentally feasible means is less explored. Here, an unusual elevation of anomalous Hall effect (AHE) is obtained in electron(Ni)-doped magnetic Weyl semimetal Co3-xNixSn2S2, showing peak values of anomalous Hall-conductivity, Hall-angle and Hall-factor at a relatively low doping level of x = 0.11. The separation of intrinsic and extrinsic contributions to total AHE using TYJ scal…
Quantum anomalous Hall effect (QAHE) has been experimentally observed in magnetically doped topological insulators. However, ultra-low temperature (usually below 300 mK), which is mainly attributed to inhomogeneous magnetic doping, becomes a daunting challenge for potential applications. Here, a \textit{nonmagnetic}-doping strategy is proposed to produce ferromagnetism and realize QAHE in topological insulators. We numerically demonstrated that magnetic moments can be induced by nitrogen or carbon substitution in Bi$_2$Se$_3$, Bi$_2$Te$_3$, and Sb$_2$Te$_3$, but only nitrogen-doped Sb$_2$Te$_3…
We report on Cr doping effect in Mn3Sn polycrystalline films with both uniform and modulation doping. It is found that Cr doping with low concentration does not cause notable changes to the structural and magnetic properties of Mn3Sn, but it significantly enhances the anomalous Hall conductivity, particularly for modulation-doped samples at low temperature. A Hall conductivity as high as 184.8 Ω-1 cm-1 is obtained for modulation-doped samples at 50 K, in a sharp contrast to vanishingly small values for undoped samples at the same temperature. We attribute the enhancement to the change of Fermi…
Two-dimensional (2D) van der Waals (vdW) magnetic materials have attracted a lot of attention owing to the stabilization of long-range magnetic order down to atomic dimensions, and the prospect of novel spintronic devices with unique functionalities. The clarification of the magnetoresistive properties and its correlation to the underlying magnetic configurations is essential for 2D vdW-based spintronic devices. Here, the effect of Co-doping on the magnetic and magnetotransport properties of Fe3GeTe2 have been investigated. Magnetotransport measurements reveal an unusual Hall effect behavior w…
Magnetic topological materials, in which strong correlations between magnetic and electronic properties of matter, give rise to various exotic phenomena such as anomalous Hall effect (AHE), topological Hall effect (THE), and skyrmion lattice. Here, we report on the electronic, magnetic, and topological properties of Mn$_{3-\it{x}}$Fe$_{\it{x}}$Sn single crystals ($\it{x}$=0, 0.25, and 0.35). Low temperature magnetic properties have been significantly changed with Fe doping. Most importantly, we observe that large uniaxial magnetocrystalline anisotropy that is induced by the Fe doping in combin…
We theoretically study the carrier doping effect for magnetism in a stacked-kagome system $\rm{{Co}_3{Sn}_2{S}_2}$ based on an effective model and the Hartree-Fock method. We show the electron filling and temperature dependences of the magnetic order parameter. The perpendicular ferromagnetic ordering is suppressed by hole doping, wheres undoped $\rm{{Co}_3{Sn}_2{S}_2}$ shows magnetic Weyl semimetal state. Additionally, in the electron-doped regime, we find a non-collinear antiferromagnetic ordering. Especially, in the non-collinear antiferromagnetic state, by considering a certain spin-orbit …
Two-dimensional (2D) van der Waals (vdW) magnetic materials have garnered considerable attention owing to the existence of magnetic order down to atomic dimensions and flexibility towards interface engineering, offering an attractive platform to explore novel spintronic phenomena and functionalities. Understanding of the magnetoresistive properties and their correlation to the underlying magnetic configurations is essential for 2D vdW-based spintronic or quantum information devices. Among the promising candidates, vdW ferromagnet (FM) Fe3GeTe2 shows an unusual magnetotransport behavior, tunabl…
Quantum anomalous Hall effect (QAHE), which generates dissipation-less edge current without external magnetic field, is observed in magnetic-ion doped topological insulators (TIs), such as Cr- and V-doped (Bi,Sb)2Te3. The QAHE emerges when the Fermi level is inside the magnetically induced gap around the original Dirac point of the TI surface state. Although the size of gap is reported to be about 50 meV, the observable temperature of QAHE has been limited below 300 mK. We attempt magnetic-Cr modulation doping into topological insulator (Bi,Sb)2Te3 films to increase the observable temperature …
An emerging phase of matter among the class of topological materials is nodal line semimetal, possessing symmetry-protected one-dimensional gapless lines at the (or close to) the Fermi level in $k$-space. When the $k$-dispersion of the nodal line is weak, van Hove singularities generated by the almost flat nodal lines may be prone to instabilities introduced by additional perturbations such as spin-orbit coupling or magnetism. Here, we study Cr-based ferromagnetic chalcospinel compound CuCr$_2$Se$_4$ (CCS) via first-principles electronic structure methods and reveal the true origin of its diss…
Using first-principles calculation methods, we reveal a series of phase transitions as a function of electron doping in single-layer 1T$'$-MoTe$_2$ and 1T$'$-WTe$_2$ exhibiting quantum spin Hall (QSH) edge states without doping. As increasing doping, we show that a phonon mediated superconducting phase first realizes and is followed by a charge density wave (CDW) phase with a nonsymmorphic lattice symmetry. The newly found CDW phase exhibits Dirac or Weyl energy bands with a spin-orbit coupling in case of a fractional band filling and re-enters into topological insulating phase with fully fill…
Stanene is a quantum spin hall insulator and a promising material for electronic and optoelectronic devices. Density functional theory (DFT) calculations are performed to study the band gap opening in stanene by elemental mono- (B, N) and co-doping (B-N). Different patterned B-N co-doping is studied to change the electronic properties in stanene. A patterned B-N co-doping opens the band gap in stanene and the semiconducting nature persists with strain. Molecular dynamics (MD) simulations are performed to confirm the thermal stability of such doped system. The stress-strain study indicates that…
As spintronic devices become more and more prevalent, the desire to find Pt free materials with large spin Hall effects is increasing. Previously it was shown that Beta W, the metastable A15 structured variant of pure W, has charge-spin conversion efficiencies on par with Pt, and it was predicted that Beta W(Ta) alloys should be even more efficient. Here we demonstrate the enhancement of the spin Hall ratio (SHR) in A15-phase Beta W films doped with Ta (W(4-x)Tax where x is between 0.28 and 0.4, deposited at room temperature using DC magnetron co-sputtering. In close agreement with theoretical…
Ferroelectric Rashba semiconductors (FERSC) have recently emerged as a promising class of spintronics materials. The peculiar coupling between spin and polar degrees of freedom responsible for several exceptional properties, including ferroelectric switching of Rashba spin texture, suggests that the electron's spin could be controlled by using only electric fields. In this regard, recent experimental studies revealing charge-to-spin interconversion phenomena in two prototypical FERSC, GeTe and SnTe, appear extremely relevant. Here, by employing density functional theory calculations, we invest…
The quantum anomalous Hall (QAH) insulator is a topological quantum state with quantized Hall resistance and zero longitudinal resistance in the absence of an external magnetic field. The QAH insulator carries spin-polarized dissipation-free chiral edge current and thus provides a unique opportunity to develop energy-efficient transformative information technology. Despite promising advances on the QAH effect over the past decade, the QAH insulator has thus far eluded any practical applications. In addition to its low working temperature, the QAH state in magnetically doped topological insulat…
Evolution of transport properties of BaFe2-xRuxAs2 in a wide range of isovalent Ru substitution
通过测量高质量BaFe_（2-x）Ru_xAs_2单晶的电阻率和霍耳系数，研究了在较宽掺杂范围内（0 < x < 1.4），Ru在Fe位上的等效替代效应。Ru取代削弱了反铁磁（AFM）序，对于0.4 < x < 0.9的相对高的掺杂水平诱导超导性。在AFM相边界附近，输运性质表现为非费米液体性质，电阻率随温度呈线性变化，霍尔系数随温度呈强的温度依赖性，并随温度变化而变化.然而，在更高的掺杂，他们都恢复传统的费米液体行为。强掺杂的霍尔系数的依赖性与一个小的磁阻表明，异常的传输特性可以解释在各向异性载流子散射由于带间AFM波动，而不是一个传统的多带的情况。
In a time-reversal invariant system, while the anomalous Hall effect identically vanishes in the linear response regime due to the constraint of time-reversal symmetry on the distribution of Berry curvature, a nonlinear Hall effect can emerge in the second-order response regime if the inversion symmetry is broken to allow a nonzero Berry curvature dipole (BCD) on the Fermi surface. In this work, we study the nonlinear Hall effect of the BCD origin in two-dimensional doped insulators and semimetals belonging to the symmetry class AI which has spinless time-reversal symmetry. Despite that the cl…
We report on the growth and characterization of Ge-doped \b{eta}-Ga2O3 thin films using a solid germanium source. \b{eta}-Ga2O3 thin films were grown using a low-pressure chemical vapor deposition (LPCVD) reactor with either an oxygen or gallium delivery tube. Films were grown on 6 degree offcut sapphire and (010) \b{eta}-Ga2O3 substrates with growth rates between 0.5 - 22 μm/hr. By controlling the germanium vapor pressure, a wide range of Hall carrier concentrations between 10^17 - 10^19 cm-3 were achieved. Low-temperature Hall data revealed a difference in donor incorporation depending on th…
