Evidence for large electric polarization from collinear magnetism in TmMnO3
V. Yu. Pomjakushin, M. Kenzelmann, A. Donni, A. B. Harris, T. Nakajima, S. Mitsuda, M. Tachibana, L. Keller, J. Mesot, H. Kitazawa, E. Takayama-Muromachi
There has been tremendous research activity in the field of magneto-electric (ME) multiferroics after Kimura et al. [1] showed that antiferromagnetic and ferroelectric order coexist in orthorhom- bically distorted perovskite TbMnO3 and are strongly coupled. It is now generally accepted that ferroelectricity in TbMnO3 is induced by magnetic long range order that breaks the symmetry of the crystal and creates a polar axis [2]. One remaining key question is whether magnetic order can induce ferroelectric polarization that is as large as that of technologically useful materials. We show that ferroelectricity in orthorhombic (o) TmMnO3 is induced by collinear magnetic order, and that the lower limit for its electric polarization is larger than in previously investigated orthorhombic heavy rare-earth manganites. The temperature dependence of the lattice constants provides fur- ther evidence of large spin-lattice coupling effects. Our experiments suggest that the ferroelectric polarization in the orthorhombic perovskites with commensurate magnetic ground states could pass the 1 microC/cm2 threshold, as suggested by theory [3, 4].
We performed comparative analysis for DFT+$U$ functionals to better understand their applicability to non-collinear magnetism. Taking LiNiPO$_4$ and Sr$_2$IrO$_4$ as examples, we investigated the results out of two formalisms based on charge-only density and spin density functional plus $U$ calculations. Our results show that the ground state spin order in terms of tilting angle is strongly dependent on Hund $J$. In particular, the opposite behavior of canting angles as a function of $J$ is found for LiNiPO$_4$. The dependence on the other physical parameters such as Hubbard $U$ and Slater par…
A canonical band theory of non-collinear magnetism is developed and applied to the close packed fcc and bcc crystal structures. Several examples of non-collinear magnetism in the periodic table are seen to be canonical in origin. This is a parameter free theory where the crystal and magnetic symmetry, and exchange splitting, uniquely determine the electronic bands. The only contribution to the determination of magnetic stability is the change in band energy due to hybridisation resulting from spin mixing, and on this basis we are able to analyse the origin of the stability of non-collinear mag…
Using a first principles based, magnetic tight-binding total energy model, the magnetization energy and moments are computed for various ordered spin configurations in the high pressure polymorphs of iron (fcc, or $γ$-Fe, and hcp, or $ε$-Fe), as well ferromagnetic bcc iron ($α$-Fe). For hcp, a non-collinear, antiferromagnetic, spin configuration that minimizes unfavorable ferromagnetic nearest neighbor ordering is the lowest energy state and is more stable than non-magnetic $ε$ iron up to about 75 GPa. Accounting for non-collinear magnetism yields better agreement with the experimental equatio…
Using results of the band structure calculations in the local-spin-density approximation we demonstrate how the crystal distortions affect the magnetic structure of orthorhombically distorted perovskites leading to a non-collinear spin arrangement. Our results suggest that the non-collinearity of the spin magnetic moments, being generally small in La$M$O$_3$ series with $M$=Cr-Fe, is large in SrRuO$_3$.
A description of non-collinear magnetism in the framework of spin-density functional theory is presented for the exact exchange energy functional which depends explicitly on two-component spinor orbitals. The equations for the effective Kohn-Sham scalar potential and magnetic field are derived within the optimized effective potential (OEP) framework. With the example of a magnetically frustrated Cr monolayer it is shown that the resulting magnetization density exhibits much more non-collinear structure than standard calculations. Furthermore, a time-dependent generalization of the non-collinea…
AMX$_3$ compounds are structurally diverse, a notable example being the post-perovskite structure which adopts a two-dimensional framework with corner- and edge-sharing octahedra. Few molecular post-perovskites are known and of these, none have reported magnetic structures. Here we report the synthesis, structure and magnetic properties of molecular post-perovskites: CsNi(NCS)$_3$, a thiocyanate framework, and two new isostructural analogues CsCo(NCS)$_3$ and CsMn(NCS)$_3$. Magnetisation measurements show that all three compounds undergo magnetic order. CsNi(NCS)$_3$ (Curie temperature, $T_\ma…
Magnetism is a key driving force controlling several thermodynamic and kinetic properties of Fe-Cr systems. We present a newly-developed TB model for Fe-Cr, where magnetism is treated beyond the usual collinear approcimation. A major advantage of this model consists in a rather simple fitting procedure. In particular, no specific properties of the binary system is explicitly required in the fitting database. The present model is proved to be accurate and highly transfer-able for electronic, magnetic and energetic properties of a large variety of structural and chemical environments: surfaces, …
How does magnetism behave when the physical dimension is reduced to the size of nanostructures? The multiplicity of magnetic states in these systems can be very rich, in that their properties depend on the atomic species, the cluster size, shape and symmetry or choice of the substrate. Small variations of the cluster parameters may change the properties dramatically. Research in this field has gained much by the many novel experimental methods and techniques exhibiting atomic resolution. Here I review the ab-initio approach, focusing on recent calculations on magnetic frustration and occurrenc…
Recent experiments showed that Co undergoes a phase transition from ferromagnetic hcp phase to non-magnetic fcc one around 100 GPa. Since the transition is of first order, a certain region of co-existence of the two phases is present. By means of \textit{ab initio} calculations, we found that the hcp phase itself undergoes a series of electronic topological transitions (ETTs), which affects both elastic and magnetic properties of the material. Most importantly, we propose that the sequence of ETTs lead to the stabilisation of a non-collinear spin arrangement in highly compressed hcp Co. Detail…
A combined experimental, using X-ray Magnetic Circular Dichroism and theoretical investigation, using full-potential Korringa-Kohn-Rostoker (KKR) Green function method, is carried out to study the spin structure of small magnetic Cr adatom--clusters on the surface of 3 monolayers of $fcc$ Fe deposited on Cu(001). The exchange interaction between the different Cr adatoms as well as between the Cr atoms and the Fe atoms is of antiferromagnetic nature and of comparable magnitude, leading due to frustration to complex non-collinear magnetic configurations. The presence of non-collinear magnetic co…
Interfaces between correlated complex oxides are promising avenues to realize new forms of magnetism that arise as a result of charge transfer, proximity effects and locally broken symmetries. We report upon the discovery of a non-collinear magnetic structure in superlattices of the ferromagnetic metallic oxide La2/3Sr1/3MnO3 (LSMO) and the correlated metal LaNiO3 (LNO). The exchange interaction between LSMO layers is mediated by the intervening LNO, such that the angle between the magnetization of neighboring LSMO layers varies in an oscillatory manner with the thickness of the LNO layer. The…
Photoinduced Odd- and Mixed-Parity Magnetism in Collinear Antiferromagnets
School of Physics, Northwest University（西北大学物理学院）；Institute of Modern Physics, Northwest University（西北大学现代物理研究所）；School of physics and astronomy, Beijing Normal University（北京师范大学物理与天文学院）；College of Materials Science and Engineering, Changsha University of Science & Technology（长沙理工大学材料科学与工程学院）
Edge non-collinear magnetism in nanoribbons of Fe3GeTe2 and Fe3GaTe2
Instituto de Física, Universidade Federal Fluminense（弗鲁米嫩塞联邦大学物理研究所）；Department of Physics and Astronomy, Uppsala University（乌普萨拉大学物理与天文学系）；School of Science and Technology, Örebro University（厄勒布鲁大学理学院）
The orthoperovskites TbCoO$_3$ and DyCoO$_3$ with Co$^{3+}$ in a non-magnetic low-spin state have been investigated by neutron diffraction down to 0.25 K. Magnetic ordering is evidenced below $T_N=3.3$ K and 3.6 K, respectively, and the ordered arrangements are of canted type, A$_x$G$_y$ for TbCoO$_3$ and G$_x$A$_y$ for DyCoO$_3$ in Bertaut's notation. The experiments are confronted with the first-principle calculations of the crystal field and magnetism of Tb$^{3+}$ and Dy$^{3+}$ ions, located in the $Pbnm$ structure on sites of $C_s$ point symmetry. Both these ions exhibit an Ising behavior,…
We present the magnetic structure of the itinerant monoarsenide, FeAs, with the B31 structure. Powder neutron diffraction confirms incommensurate modulated magnetism with wavevector $\mathbf{q} = (0.395\pm0.001)\mathbf{c}^*$ at 4 K, but cannot distinguish between a simple spiral and a collinear spin-density wave structure. Polarized single crystal diffraction confirms that the structure is best described as a non-collinear spin-density wave arising from a combination of itinerant and localized behavior with spin amplitude along the b-axis direction being (15 $\pm$ 5)% larger than in the a-dire…
The development of quantitative models for radiation damage effects in iron, iron alloys and steels, particularly for the high temperature properties of the alloys, requires understanding of magnetic interactions, which control the phase stability of ferritic-martensitic, ferritic, and austenitic steels. In this work, disordered magnetic configurations of pure iron and Fe-Cr alloys are investigated using Density Functional Theory (DFT) formalism, in the form of constrained non-collinear magnetic calculations, with the objective of creating a database of atomic magnetic moments and forces actin…
We study the non-collinear exchange coupling across a trilayer magnetic junction consisting of two ferromagnets separated by a thin dilute magnetic semiconductor containing itinerant carriers with finite spin relaxation. It is remarkable that, by increasing the spin relaxation, the critical temperature is substantially enhanced and the shape of the magnetization curve becomes more mean-field like. We attribute these interesting changes to the broken time-reversal symmetry which suppresses the oscillatory Ruderman-Kittel-Kasuya-Yosida interaction. Our argument is further strengthened by the eme…
We have studied the electronic, magnetic and linear phonon dispersion behavior of Phosphorene monolayer using rst principle based ab initio method. Phosphorene monolayer is a semiconducting system with a dimensional dependent variable range of band gap. Vacancy has been done to study the geometry and physical behavior of the monolayer system. Pristine, vacancy induced monolayer and vacancy induced doped monolayer are included in the calculation. Dopant concentration has been well checked via optimization algorithm to maintain the dilute magnetic semiconducting behavior of the monolayer system.…
We have carried out collinear and non-collinear electronic structure calculations to investigate the structural, electronic and magnetic properties of isolated Cr atoms, dimers and compact trimers. We find that the Cr monomer prefers to adsrob on the fcc hollow site with a binding energy of 3.13 eV and a magnetic moment of of 3.93 $μ_B$. The calculated Kondo temperature of 0.7 K for the monomer is consistent with the lack of a Kondo peak in scanning tunneling microscopy (STM) experiments at 7 K. The compact Cr dimer orders antiferromagnetically and its bond length contracts to 1.72 $Å$ close t…
The link between the crystal distortions of the perovskite structure and the magnetic exchange interaction, the single-ion anisotropy (SIA) and the Dzyaloshinsky-Moriya (DM) interaction are investigated by means of density-functional calculations. Using BiFeO$_3$ and LaFeO$_3$ as model systems, we quantify the relationship between the oxygen octahedra rotations, the ferroelectricity and the weak ferromagnetism (wFM). We recover the fact that the wFM is due to the DM interaction induced by the oxygen octahedra rotations. We find a simple relationship between the wFM, the oxygen rotation amplitu…
The magnetic and electrical properties of Co$_3$TeO$_6$ single-crystals with corundum related structure reveal a magnetic-field induced polarization below 21 K. A sharp peak in the specific heat at \approx 18 K indicates a reconstructive-type first-order phase transition. From second-harmonic generation (SHG) measurements breaking of inversion symmetry is evident and the point-group symmetry was determined as m. The temperature and magnetic-field dependence of the magnetic and electrical polarizations are discussed in the light of the SHG results.
We present a microscopic theory that shows the importance of spin-orbit coupling in perovskite compounds with heavy ions. In BiFeO3 (BFO) the spin-orbit coupling at the bismuth ion sites results in a special kind of magnetic anisotropy that is linear in the applied E-field. This interaction can convert the cycloid ground state into a homogeneous antiferromagnet, with a weak ferromagnetic moment whose orientation can be controlled by the E-field direction. Remarkably, the E-field control of magnetism occurs without poling the ferroelectric moment, providing a pathway for reduced energy dissipat…
Magnetism in single-side hydrogenated (C$_2$H) and fluorinated (C$_2$F) graphene is analyzed in terms of the Heisenberg model with parameters determined from first principles. We predict a frustrated ground state for both systems, which means the instability of collinear spin structures and sheds light on the absence of a conventional magnetic ordering in defective graphene demonstrated in recent experiments. Moreover, our findings suggest a highly correlated magnetic behavior at low temperatures offering the possibility of a spin-liquid state.
Multiferroic materials, with their combined and coupled magnetism and ferroelectricity, providea playground for studying new physics and chemistry as well as a platform for development ofnovel devices and technologies. Based on my July 2017 Royal Society Inaugural Lecture, I review recent progress and propose future directions in the fundamentals and applications of multiferroics, with a focus on unanticipated developments outside of the core activity of electric-field control of magnetism.
We report a new peculiar effect of the interaction between a sublattice of frustrated quantum spin-1/2 chains and a sublattice of pseudospin-1/2 centers (quantum electric dipoles) uniquely co-existing in the complex oxide Li2ZrCuO4. 7Li nuclear magnetic-, Cu2+ electron spin resonance and a complex dielectric constant data reveal that the sublattice of Li+-derived electric dipoles orders glass like at Tg ~ 70 K yielding a spin site nonequivalency in the CuO2 chains. We suggest that such a remarkable interplay between electrical and spin degrees of freedom might strongly influence the properties…
Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Institute of Physics, Czech Academy of Sciences（捷克科学院物理研究所）
Recent experiments on Pd$_{3}$Fe intermetallics [Phys. Rev. Lett. 102, 237202 (2009)] have revealed that the system behaves like a classical invar alloy under high pressure. The experimental pressure-volume relation suggests an anomalous volume collapse and a substantial increase in bulk modulus around the pressure where invar behavior is observed. With the help of first-principles density functional theory based calculations, we have explored various magnetic phases (ferromagnetic, fully and partially disordered local moment, spin spiral) in order to understand the effect of pressure on magne…
Correlation between magnetism and the Verwey transition in magnetite
AGH University of Krakow（克拉科夫AGH科技大学）；Institute of Solid State Physics, TU Wien（维也纳工业大学固体物理研究所）；Mössbauer Spectroscopy Laboratory, Institute of Technology, University of the National Education Commission（国家教育委员会理工学院穆斯堡尔谱学实验室）；The Henryk Niewodniczanski Institute of Nuclear Physics, Polish Academy of Sciences（波兰科学院亨利克·涅沃德尼察斯基核物理研究所）；Purdue University（普渡大学）；Univ. Grenoble Alpes（格勒诺布尔阿尔卑斯大学）；Institut Néel, CNRS & Univ. Grenoble Alpes（内尔研究所，法国国家科学研究中心与格勒诺布尔阿尔卑斯大学）；University of Zagreb（萨格勒布大学）
In this paper, we report the results of an ambient and high pressure study of a 5f-electron ferromagnet URhGa. The work is focused on measurements of magnetic and thermodynamic properties of a single crystal sample and on the construction of the p-T phase diagram. Diamond anvil cells were employed to measure the magnetization and electrical resistivity pressures up to ~ 9 GPa. At ambient pressure, URhGa exhibits collinear ferromagnetic ordering of uranium magnetic moments μU ~ 1.1 μB (at 2 K) aligned along the c-axis of the hexagonal crystal structure below the Curie temperature TC = 41K. With…
In the metallic pyrochlore Nd$_2$Mo$_2$O$_7$, the conducting Molybdenum sublattice adopts canted, yet nearly collinear ferromagnetic order with nonzero scalar spin chirality. The chemical potential may be controlled by replacing Nd$^{3+}$ with Ca$^{2+}$, while introducing only minimal additional disorder to the conducting states. Here, we demonstrate the stability of the canted ferromagnetic state, including the tilting angle of Molybdenum spins, in (Nd$_{1-x}$Ca$_{x}$)$_2$Mo$_2$O$_7$ (NCMO) with $x\le 0.15$ using magnetic susceptibility measurements. Mo-Mo and Mo-Nd magnetic couplings both ch…
This review article aims at illustrating the recent progresses in the electrical control of magnetism in oxides with profound physics and enormous potential applications. In the first part, we provide a comprehensive summary of the electrical control of magnetism in the classic multiferroic heterostructures and clarify their various mechanisms lying behind. The second part focuses on the novel route of electric double layer gating for driving a significantly electronic phase transition in magnetic oxides by a small voltage. The electric field applied on the ordinary dielectric oxide in the thi…
Electric susceptibility of antiferromagnetic multiferroics with cycloidal spin order at magnetoelectric effect associated with collinear component of spins
Sr$_{3}$ZnIrO$_{6}$ is an effective spin one-half Mott insulating iridate belonging to a family of magnets which includes a number of quasi-one dimensional systems as well as materials exhibiting three dimensional order. Here we present the results of an extensive investigation into the magnetism including heat capacity, a.c. susceptibility, muon spin rotation ($μ$SR), neutron diffraction and inelastic neutron scattering on the same sample. It is established that the material exhibits a transition at about $17$ K into a three-dimensional antiferromagnetic structure with propagation vector $\bo…
We study theoretically the RKKY interaction between magnetic impurities on the surface of three-dimensional topological insulators, mediated by the helical Dirac electrons. Exact analytical expression shows that the RKKY interaction consists of the Heisenberg-like, Ising-like and DM-like terms. It provides us a new way to control surface magnetism electrically. The gap opened by doped magnetic ions can lead to a short-range Bloembergen-Rowland interaction. The competition among the Heisenberg, Ising and DM terms leads to rich spin configurations and anomalous Hall effect on different lattices.
Through systematics density functional calculations, the mechanism of the substrate induced spin reorientation transition in FePc/O-Cu(110) was explained in terms of charge transfer and rearrangement of Fe-d orbitals. Moreover, we found giant magnetoelectric effects in this system, manifested by the sensitive dependences of its magnetic moment and magnetic anisotropy energy on external electric field. In particular, the direction of magnetization of FePc/O-Cu(110) is switchable between in-plane and perpendicular axes, simply by applying an external electric field of 0.5 eV/Å along the surface …
We investigated the electronic and magnetic properties of the pyrochlore oxide Cd$_2$Os$_2$O$_7$ using the density-functional theory plus on-site repulsion ($U$) method, and depict the ground-state phase diagram with respect to $U$. We conclude that the all-in/all-out non-collinear magnetic order is stable in a wide range of $U$. We also show that the easy-axis anisotropy arising from the spin-orbit (SO) coupling plays a significant role in stabilizing the all-in/all-out magnetic order. A \textit{pseudo gap} was observed near the transition between the antiferromagnetic metallic and insulating…
Using a first principles density functional electronic structure method, we study the energy gaps and magnetism in bilayer graphene nanoribbons as a function of the ribbon width and the strength of an external electric field between the layers. We assume AB (Bernal) stacking and consider both armchair and zigzag edges and two edge alignments distinguished by a 60$^o$ rotation of one layer with respect to the other. Armchair ribbons exhibit three classes of bilayer gaps which decrease with increasing ribbon width. An external electric field between the layers increases the gap in narrow ribbons…
We address the importance of the modern theory of orbital magnetization for spintronics. Based on an all-electron first-principles approach, we demonstrate that the predictive power of the routinely employed "atom-centered" approximation is limited to materials like elemental bulk ferromagnets, while the application of the modern theory of orbital magnetization is crucial in chemically or structurally inhomogeneous systems such as magnetic thin films, and materials exhibiting non-trivial topology in reciprocal and real space,~e.g.,~Chern insulators or non-collinear systems. We find that the mo…
Towards next-generation spintronics devices, such as computer memories and logic chips, it is necessary to satisfy high thermal stability, low-power consumption and high spin-polarization simultaneously. Here, from first-principles, we investigate thermal stability (both structure and magnetization) and the electric field control of magnetic anisotropy on Co2FeAl (CFA)/MgO. A phase diagram of structural thermal stability of the CFA/MgO interface is illustrated. An interfacial perpendicular-anisotropy, coming from the Fe-O orbital hybridization, provides high magnetic thermal stability and a lo…
Magnetic skyrmions are localised non-collinear spin textures with high potential for future spintronic applications. Skyrmion phases have been discovered in a number of materials and a focus of current research is the preparation, detection, and manipulation of individual skyrmions for an implementation in devices. Local experimental characterization of skyrmions has been performed by, e.g., Lorentz microscopy or atomic-scale tunnel magnetoresistance measurements using spin-polarised scanning tunneling microscopy. Here, we report on a drastic change of the differential tunnel conductance for m…
Recently intrinsic ferromagnetism in two-dimensional(2D) van der Waals materials was discovered [1, 2, 3]. A monolayer of Chromiun triiodide(CrI3) is ferromagnetic while a bilayer structure was reported to be anti-ferro magnetic, moreover an external electric field changes its magnetic phase [4]. We have studied the two found in nature stackings of CrI3 bilayers and found that indeed the magnetic phase of one of them can be tuned by an external electric field while the other remains ferromagnetic. We simulate those results with ab initio calculations and explain them with a simple model based …
Based on first principles calculations we investigate the electronic and magnetic properties of Pt layers in Pd$(001)$/Co/Pt thin film structures exposed to an external electric field. Due to the Co underlayer, the surface Pt layers have induced moments that are modified by an external electric field. The field induced changes can be explained by the modified spin-dependent orbital hybridization that varies non-linearly with the field strength. We calculate the x-ray absorption and the x-ray magnetic circular dichroism spectra for an applied external electric field and examine its impact on th…
