Exchange interactions in α- and γ-Fe are investigated within an ab-initio spin spiral approach. We have performed total energy calculations for different magnetic structures as a function of lattice distortions, related with various cell volumes and the Bain tetragonal deformations. The effective exchange parameters in γ-Fe are very sensitive to the lattice distortions, leading to the ferromagnetic ground state for the tetragonal deformation or increase of the volume cell. At the same time, the magnetic-structure-independent part of the total energy changes very slowly with the tetragonal deformations. The computational results demonstrate a strong mutual dependence of crystal and magnetic structures in Fe and explain the observable "anti-Invar" behavior of thermal expansion coefficient in γ-Fe.
Complex experimental and theoretical study of the magnetic, magnetoelectric, and magnetoelastic properties of neodymium iron borate NdFe3(BO3)4 along various crystallographic directions have been carried out in strong pulsed magnetic fields up to 230 kOe in a temperature range of 4.2-50 K. It has been found that neodymium iron borate, as well as gadolinium iron borate, is a multiferroic. It has much larger (above 3 10^(-4) C/m^2) electric polarization controlled by the magnetic field and giant quadratic magnetoelectric effect. The exchange field between the rare-earth and iron subsystems (~50 …
Pressure-induced thermal expansion anomalies in dhcp iron hydride associated with magnetoelastic coupling
The University of Tokyo（东京大学）；Yale University（耶鲁大学）；Flatiron Institute（平顿研究所）；Center for High Pressure Science and Technology Advanced Research（高压科学与技术先进研究中心）；Pohang University of Science and Technology（浦项科技大学）；Japan Synchrotron Radiation Research Institute（日本同步辐射研究所）
Magnetoelastic coupling, i.e., the change of crystal lattice induced by a spin order, is not only scientifically interesting, but also technically important. In this work, we propose a general microscopic model from first-principles calculations to describe the magnetoelastic coupling and provide a way to construct the microscopic model from density functional theory calculations. Based on this model, we reveal that there exists a previously unexpected contribution to the electric polarization induced by the spin-order in multiferroics due to the combined effects of magnetoelastic coupling and…
A method is developed which allows to determine the first-order and the second-order magnetoelastic coefficients of a magnetic bulk material from the ab-initio calculation of the magnetocrystalline anisotropy energy as function of a prestrain. Excplicit results are given for bcc Fe, and they agree well with experimental data obtained from the magnetostrictive stress measurements for epitaxial Fe films.
Many of the iron pnictides have strongly anisotropic normal-state characteristics, important for the exotic magnetic and superconducting behavior these materials exhibit. Yet, the origin of the observed anisotropy is unclear. Electronically driven nematicity has been suggested, but distinguishing this as an independent degree of freedom from magnetic and structural orders is difficult, as these couple together to break the same tetragonal symmetry. Here we use time-resolved polarimetry to reveal critical nematic fluctuations in unstrained Ba(Fe_(1-x)Co_x)_2As_2. The femtosecond anisotropic res…
We have studied the magnetodielectric and magnetoelastic coupling in TbFe3(BO3)4 single crystals by means of capacitance, magnetostriction and Raman spectroscopy measurements. The data reveal strong magnetic field effects on the dielectric constant and on the macroscopic sample length which are associated to long range magnetic ordering and a field-driven metamagnetic transition. We discuss the coupling of the dielectric, structural, and magnetic order parameters and attribute the origin of the magnetodielectric coupling to phonon mode shifts according to the Lyddane-Sachs-Teller (LST) relatio…
Analytical expressions for the magnetoelastic anisotropy constants of cubic magnetic systems are derived for rectangular and oblique distortions originating from epitaxial growth on substrates with lower crystal symmetry. In particular, the temperature variation of the magnetic properties of magnetic films grown on barium titanate (BaTiO3) substrates are explained in terms of strain-induced magnetic anisotropies caused by the temperature dependent phase transitions of BaTiO3. Our results quantify the experimental observations in ferromagnet/\bto-based structures, which have been proposed as te…
In this work, we leverage atomistic spin-lattice simulations to examine how magnetic interactions impact the propagation of sound waves through a ferromagnetic material. To achieve this, we characterize the sound wave velocity in BCC iron, a prototypical ferromagnetic material, using three different approaches that are based on the oscillations of kinetic energy, finite-displacement derived forces, and corrections to the elastic constants, respectively. Successfully applying these methods within the spin-lattice framework, we find good agreement with the Simon effect including high order terms…
Magnetoelastic coupling in stripe-domain states of yttrium iron garnet
University College London（伦敦大学学院）；Imperial College London（帝国理工学院）；Japan Atomic Energy Agency（日本原子能机构）；The University of Tokyo（东京大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所新兴物质科学中心）；WPI-Advanced Institute for Materials Research, Tohoku University（东北大学材料研究高等研究院）
We present a laterally resolved X-ray magnetic dichroism study of the magnetic proximity effect in a highly ordered oxide system, i.e. NiO films on Fe3O4(110). We found that the magnetic interface shows an ultrasharp electronic, magnetic and structural transition from the ferrimagnet to the antiferromagnet. The monolayer which forms the interface reconstructs to NiFe2O4 and exhibits an enhanced Fe and Ni orbital moment, possibly caused by bonding anisotropy or electronic interaction between Fe and Ni cations. The absence of spin-flop coupling for this crystallographic orientation can be explai…
The realization of intertwined ferroelasticity and ferromagnetism in two-dimensional (2D) lattices is of great interest for broad nanoscale applications, but still remains a remarkable challenge. Here, we propose an alternative approach to realize the strongly coupled ferromagnetism and ferroelasticity by carrier doping. We demonstrate that prototypical 2D \b{eta}-PbO is dynamically, thermally and mechanically stable. Under hole doping, 2D \b{eta}-PbO possesses ferromagnetism and ferroelasticity simultaneously. Moreover, the robustness of ferromagnetic and ferroelastic orders are doping tunabl…
We show that the magnetoelastic coupling between the magnetization and the amplitude of a short wavelength phonon enables the existence of a first order premartensitic transition from a bcc to a micromodulated phase in $Ni_{2}MnGa$. Such a magnetoelastic coupling has been experimentally evidenced by AC susceptibility and ultrasonic measurements under applied magnetic field. A latent heat around 9 J/mol has been measured using a highly sensitive calorimeter. This value is in very good agreement with the value predicted by a proposed model.
We report measurements of the in-plane magnetoelastic coupling in ultra-thin Ta|CoFeB|MgO layers as a function of uniaxial strain, conducted using a four-point bending apparatus. For annealed samples, we observe a strong dependence on the thickness of the CoFeB layer in the range 1.3-2.0 nm, which can be modeled as arising from a combination of effective surface and volume contributions to the magnetoelastic coupling. We point out that if similar thickness dependence exists for magnetoelastic coupling in response to biaxial strain, then the standard Néel model for the magnetic anisotropy energ…
Multiferroics where at least two primary ferroic orders are present and coupled in a single system constitute an important class of materials. They attracted special consideration as they present both intriguing fundamental physics problems and technological importance for potential multifunctional devices. Here, we present the evidence of multiferroicity and magnetoelectric (ME) coupling in alpha-Mn2O3; a unique binary perovskite. Corresponding to the antiferromagnetic (AFM) ordering around 80K, a clear frequency independent transition is observed in the dielectric permittivity. We showed tha…
Chiral Phonons Enable Ultrafast Magnetization Switching via Magnetoelastic Coupling
Nanjing University of Aeronautics and Astronautics (NUAA)（南京航空航天大学）；Instituto de Ciencia de Materiales de Madrid (ICMM), CSIC（马德里材料科学研究所，西班牙国家科学研究委员会）；The University of Manchester（曼彻斯特大学）；University of York（约克大学）
Clear anomalies in the lattice thermal expansion (deviation from linear variation) and elastic properties (softening of the sound velocity) at the antiferromagnetic-to-paramagnetic transition are observed in the prototypical multiferroic BiFeO3 using a combination of picosecond acoustic pump-probe and high-temperature X-ray diffraction experiments. Similar anomalies are also evidenced using first-principles calculations supporting our experimental findings. Those calculations in addition to a simple Landau-like model we also developed allow to understand the elastic softening and lattice chang…
The multiferroic properties of EuTiO3 are greatly enhanced when a sample is strained, signifying that coupling between strain and structural, magnetic or ferroelectric order parameters is extremely important. Here resonant ultrasound spectroscopy has been used to investigate strain coupling effects, as well as possible additional phase transitions, through their influence on elastic and anelastic relaxations that occur as a function of temperature between 2 and 300 K and with applied magnetic field up to 14 T. Antiferromagnetic ordering is accompanied by acoustic loss and softening, and a weak…
Temperature dependent X-ray diffraction and Raman spectroscopic studies were carried out on the flux grown single crystals of gallium ferrite with Ga:Fe ratio of 0.9:1.1. Site occupancy calculations from the Rietveld refinement of the X-ray data led to the estimated magnetic moment of ~0.60 \muB /f.u. which was in good agreement with the experimental data. Combination of these two measurements indicates that there is no structural phase transition in the material between 18 K to 700 K. A detailed line shape analysis of the Raman mode at ~375 cm^-1 revealed a discontinuity in the peak position …
Magnetoelastic and magnetoelectric coupling in the artificial multiferroic heterostructures facilitate valuable features for device applications such as magnetic field sensors and electric write magnetic-read memory devices. In a ferromagnetic/ferroelectric heterostructures, the strain mediated coupling exploits piezoelectricity/electrostriction in ferroelectric phase and magnetostriction/piezomagnetism in ferromagnetic phase. Such verity of these combined effect can be manipulated by an external perturbation, such as electric field, temperature or magnetic field. Here, we demonstrate the remo…
We theoretically investigate the magnetoelastic coupling (MEC) and its effect on magnon transport in two-dimensional antiferromagnets with a honeycomb lattice. MEC coeffcient along with magnetic exchange parameters and spring constants are computed for monolayers of transition metal trichalcogenides with Néel order ($\text{MnPS}_3$ and $\text{VPS}_3$) and zigzag order ($\text{CrSiTe}_3$, $\text{NiPS}_3$ and $\text{NiPSe}_3$) by $ab$ $initio$ calculations. Using these parameters, we predict that the spin-Nernst coefficient is significantly enhanced due to magnetoelastic coupling. Our study show…
We have performed a study of the magnetic, magnetoelastic, and corrosion resistance properties of seven different composition magnetoelastic-resonant platforms. For some applications, such as structural health monitoring, these materials must have not only good magnetomechanical properties, but also a high corrosion resistance. In the fabricated metallic glasses of composition Fe(73-x)NixCr5Si10B12, the Fe/Ni ratio was varied (Fe + Ni = 73% at.) thus changing the magnetic and magnetoelastic properties. A small amount of chromium (Cr5) was added in order to achieve the desired good corrosion re…
The physical properties of the spinel LiGaCr4S8 have been studied with neutron diffraction, X-ray diffraction, magnetic susceptibility and heat capacity measurements. The neutron diffraction and synchrotron X-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First principles calculations find a strong coupling between the lattice and the simulated mag…
Microscopic spin interactions on a deformed Kagomé lattice of volborthite are investigated through magnetoelastic couplings. A negative longitudinal magnetostriction $ΔL<0$ in the $b$ axis is observed, which depends on the magnetization $M$ with a peculiar relation of $ΔL/L \propto M^{1.3}$. Based on the exchange striction model, it is argued that the negative magnetostriction originates from a pantograph-like lattice change of the Cu-O-Cu chain in the $b$ axis, and that the peculiar dependence arises from the local spin correlation. This idea is supported by DFT+$U$ calculations simulating th…
The influence of epitaxial strain on uniaxial magnetic anisotropy of Co$_{2}$FeSi (CFS) and Co$_{2}$MnSi (CMS) Heusler alloy thin films grown on (001) SrTiO$_3$ (STO) and MgO is reported. The in-plane biaxial strain is susceptible to tune by varying the thickness of the films on STO, while on MgO the films show in-plane easy axis for magnetization (\overrightarrow{M}) irrespective of their thickness. A variational analysis of magnetic free energy functional within the Stoner-Wohlfarth coherent rotation model with out-of-plane uniaxial anisotropy for the films on STO showed the presence of magn…
Magnetoelastic Waves in Ferromagnetic Thin Films Mediated by Dipolar Interactions
Institute of Science Tokyo（东京科学大学）；The University of Tokyo（东京大学）；NTT, Inc.（日本电报电话公司）；Japan Atomic Energy Agency（日本原子能研究开发机构）；RIKEN（理化学研究所）；Hiroshima University（广岛大学）
Our measured dielectric constant and mechanical response of multiferroic BiFeO3 indicate four phase transitions below room temperature. Features correlate with those reported at 50K (from a peak in the zero-field-cooled magnetic susceptibility) and 230K (from splitting between field-cooled and zero-field-cooled magnetic data[1], and 200K (from magnon light scattering cross sections[2]). The primary order parameter is not the polarization in any of the low-T transitions. Instead, the transition near 230 K shows strong elastic coupling, while that at 50K is fundamentally magnetic, but magnetostr…
Thermodynamic description of a model system with magnetoelastic coupling is presented. The elastic, vibrational, electronic and magnetic energy contributions are taken into account. The long-range RKKY interaction is considered together with the nearest-neighbour direct exchange. The generalized Gibbs potential and the set of equations of state are derived, from which all thermodynamic functions are self-consistently obtained. Thermodynamic properties are calculated numerically for FCC structure for arbitrary external pressure, magnetic field and temperature, and widely discussed. In particula…
Extrinsic multiferroic hybrid structures consisting of ferromagnetic and ferroelectric layers elastically coupled to each other are promising due to their robust magnetoelectric effects even at room temperature. For a quantitative analysis of these magnetoelectric effects, a detailed knowledge of the piezoelectric and magnetoelastic behavior of both constituents as well as their mutual elastic coupling is mandatory. We here report on a theoretical and experimental study of the magnetic behavior of BaTiO3-based extrinsic multiferroic structures. An excellent agreement between molecular dynamics…
Low temperature magnetic and structural behavior of the extended Kagome system YBaCo4O7 has been studied by single crystal neutron diffraction and high-resolution powder X-ray diffraction. Long-range magnetic ordering associated with a structural transition from orthorhombic Pbn2_1 to monoclinic P2_1 symmetry has been found at T_1 ~ 100 K. The interplay between the structural and magnetic degrees of freedom testifies that the degeneracy of the magnetic ground state, present in the orthorhombic phase, is lifted through a strong magnetoelastic coupling, as observed in other frustrated systems. A…
In the paper a study of a model magnetoelastic solid system is presented. The system of interest is a mean-field magnet with nearest-neighbour ferromagnetic interactions and the underlying s.c. crystalline lattice with the long-range Morse interatomic potential and the anharmonic Debye model for the lattice vibrations. The influence of the external magnetic field on the thermodynamics is investigated, with special emphasis put on the consequences of the magnetoelastic coupling, introduced by the power-law distance dependence of the magnetic exchange integral. Within the fully self-consistent, …
Using a magneto-optical pump-probe technique with micrometer spatial resolution we show that magnetization precession can be launched in individual magnetic domains imprinted in a Co$_{40}$Fe$_{40}$B$_{20}$ (CoFeB) layer by elastic coupling to ferroelectric domains in a BaTiO$_{3}$ substrate. The dependence of the precession parameters on external magnetic field strength and orientation reveal that by laser-induced ultrafast partial quenching of the magnetoelastic coupling parameter of CoFeB by $\approx$27% along with 10% ultrafast demagnetization trigger the magnetization precession. The rela…
Tetragonal CuMnAs was the first antiferromagnet where reorientation of the Néel vector was reported to occur by an inverse spin galvanic effect. A complicating factor in the formation of phase-pure tetragonal CuMnAs is the formation of an orthorhombic phase with nearly the same stoichiometry. Pure-phase tetragonal CuMnAs has been reported to require an excess of Cu to maintain a single phase in traditional solid state synthesis reactions. Here we show that subtle differences in diffraction patterns signal pervasive inhomogeneity and phase separation, even in Cu-rich Cu$_{1.18}$Mn$_{0.82}$As. F…
Kinetics of polymorphous "gamma"-"alfa" transformation in Fe is studied numerically within a model taking into account both lattice and magnetic degrees of freedom, based on first-principle calculations of the total energy for different magnetic states. It is shown that magnetoelastic phenomena, namely, a strong sensitivity of the potential relief along the Bain deformation path to the magnetic state, are crucial for the picture of the transformation. With the temperature increase, a scenario of the phase transformation evolves from a homogeneous lattice instability at T<Ms (Ms is the temperat…
Emergence of multiple quasi-ferromagnetic magnon modes induced by strong magnetoelastic coupling in $TmFeO_3$ single crystal
Johannes Gutenberg University Mainz（约翰内斯·古腾堡美因茨大学）；Shanghai University（上海大学）；Shanghai Jiao Tong University（上海交通大学）；Norwegian University of Science and Technology（挪威科技大学）
Perpendicular magnetic anisotropy (PMA) is a necessary condition for many spintronic applications like spin-orbit torques switching, logic and memory devices. An important class of magnetic insulators with low Gilbert damping at room temperature are iron garnets, which only have a few PMA types such as terbium and samarium iron garnet. More and stable PMA garnet options are necessary for researchers to be able to investigate new spintronic phenomena. In this study, we predict 20 new substrate/magnetic iron garnet film pairs with stable PMA at room temperature. The effective anisotropy energies…
Using spin-wave tomography (SWaT), we have investigated the excitation and the propagation dynamics of optically-excited magnetoelastic waves, i.e. hybridized modes of spin waves and elastic waves, in a garnet film. By using time-resolved SWaT, we reveal the excitation dynamics of magnetoelastic waves through coherent-energy transfer between optically-excited pure-elastic waves and spin waves via magnetoelastic coupling. This process realizes frequency and wavenumber selective excitation of spin waves at the crossing of the dispersion relations of spin waves and elastic waves. Finally, we demo…
We present a comprehensive first principles electronic structure study of the magnetoelastic and magnetostrictive properties in the Co-based Co$_2$XAl (X = V, Ti, Cr, Mn, Fe) full Heusler compounds. In addition to the commonly used total energy approach, we employ torque method to calculate the magnetoelastic tensor elements. We show that the torque based methods are in general computationally more efficient, and allow to unveil the atomic- and orbital-contributions to the magnetoelastic constants in an exact manner, as opposed to the conventional approaches based on second order perturbation …
Single-crystal synchrotron x-ray diffraction studies of CeFeAsO reveal strong anisotropy in the charge correlation lengths along or perpendicular to the in-plane antiferromagnetic (AFM) wave-vector at low temperatures, indicating an anisotropic two-dimensional magnetoelastic coupling. The high-resolution setup allows to distinctly monitor each of the twin domains by virtue of a finite misfit angle between them that follows the order parameter. In addition, we find that the in-plane correlations, above the orthorhombic (O)-to-tetragonal (T) transition, are shorter than those in each of the doma…
Hexagonal YMnO_3 with space group P63cm is one of the rare examples of multiferroic materials that exhibit co-dependence of a robust ferroelectric phase along with antiferromagnetic ordering. This is primarily ascribed to tilting of the MnO_5 polyhedra driven by magnetoelectric coupling. We report on the effect of magnetic field at the atomic level in YMnO_3 by utilizing magnetic field and temperature dependent neutron diffraction measurements. We show that near the Néel temperature the lattice parameters, effective magnetic moment per site, Mn-O bond lengths and O-Mn-O bond angles show large …
High-quality single crystals of CoTiO$_3$ are grown and used to elucidate in detail structural and magnetostructural effects by means of high-resolution capacitance dilatometry studies in fields up to 15 T which are complemented by specific heat and magnetization measurements. In addition, we refine the single-crystal structure of the ilmenite ($R\bar{3}$) phase. At the antiferromagnetic ordering temperature $T_\mathrm{N}$, pronounced $λ$-shaped anomaly in the thermal expansion coefficients signals shrinking of both the $c$ and $b$ axes, indicating strong magnetoelastic coupling with uniaxial …
Quantification of electronic and magnetoelastic mechanisms of first-order magnetic phase transitions from first principles: application to caloric effects in La(Fe$_x$Si$_{1-x}$)$_{13}$
Giant spin Nernst effect in a two-dimensional antiferromagnet due to magnetoelastic coupling-induced gaps and interband transitions between magnon-like bands
For disordered Heisenberg systems with small single ion anisotropy, two spin glass transitions below the long range ordered phase transition temperature has been predicted theoretically for compositions close to the percolation threshold. Experimental verification of these predictions is still controversial for conventional spin glasses. We show that multiferroic spin glass systems can provide a unique platform for verifying these theoretical predictions via a study of change in magnetoelastic and magnetoelectric couplings, obtained from an analysis of diffraction data, at the spin glass trans…
When magnons and phonons, the fundamental quasiparticles of the solid, are coupled to one another, they form a new hybrid quasi-particle, leading to novel phenomena and interesting applications. Despite its wide-ranging importance, however, detailed experimental studies on the underlying Hamiltonian is rare for actual materials. Moreover, the anharmonicity of such magnetoelastic excitations remains largely unexplored although it is essential for a proper understanding of their diverse thermodynamic behaviour as well as intrinsic zero-temperature decay. Here we show that in noncollinear antifer…
Extensive magnetization and magnetostriction measurements were carried out on a single crystal of GdNi2B2C along the main tetragonal axes. Within the paramagnetic phase, the magnetic and strain susceptibilities revealed a weak anisotropy in the exchange couplings and two-ion tetragonal-preserving alpha-strain modes. Within the ordered phase, magnetization and magnetostriction revealed a relatively strong orthorhombic distortion mode and rich field-temperature phase diagrams. For H//(100) phase diagram, three field-induced transformations were observed, namely, at: Hd(T), related to the domain …
Magnetoelastic Transport-Path Reconstruction and Giant Magnetotransport Responses in a Two-Dimensional Antiferromagnet
Key Laboratory of Materials Physics, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences（中国科学院合肥物质科学研究院固体物理研究所材料物理重点实验室）；University of Science and Technology of China（中国科学技术大学）；School of Physics, University of Electronic Science and Technology of China（电子科技大学物理学院）；Anhui Key Laboratory of Low-Energy Quantum Materials and Devices, High Magnetic Field Laboratory, HFIPS, Chinese Academy of Sciences（中国科学院合肥物质科学研究院高磁场科学中心安徽省低能量子材料与器件重点实验室）；Collaborative Innovation Center of Microstructures, Nanjing University（南京大学微观结构协同创新中心）；Department of Physics and Astronomy & Nebraska Center for Materials and Nanoscience, University of Nebraska（内布拉斯加大学物理与天文学系及内布拉斯加材料与纳米科学中心）；State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences（中国科学院半导体研究所半导体物理与芯片技术国家重点实验室）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学材料科学与光电工程学院）
The exchange bias at ferromagnetic/antiferromagnetic interfaces strongly depends upon the state of antiferromagnetic (AF) layer which, due to strong magnetoelastic coupling, is sensitive to mechanical stresses. In the present paper we consider magnetoelastic effects that arise at FM/AF interface due to lattice misfit and magnetic ordering. We show how magnetostriction affects mutual orientation of AF and FM vectors and easy-axis direction in thin AF layer. The results obtained could be used for tailoring exchange biased systems.
