Dynamical magnetic susceptibility of non-collinear magnets: A novel KKR-based ab initio scheme and its application
Institute for Theoretical Physics, Johannes Kepler University Linz（林茨约翰内斯开普勒大学理论物理研究所）；Hamburg University of Applied Sciences（汉堡应用科学大学）；Max Planck Institute of Microstructure Physics（马克斯·普朗克微结构物理研究所）；Donostia International Physics Center (DIPC)（多诺斯蒂亚国际物理中心）
A novel implementation of the linear response time-dependent density functional theory addressing spin excitations in non-collinear magnets based on the Korringa-Kohn-Rostoker Green's function method is presented. Following the exposition of the formalism based on the adiabatic local spin density approximation to the exchange-correlation kernel generalized to the noncollinear case, the computational scheme is discussed in detail. The formation of the Goldstone modes in non-collinear susceptibility calculations is elaborated on formally and from the numerical convergence point of view. The scheme is deployed to study the dispersion and Landau damping of magnons in the altermagnetic non-collinear kagome antiferromagnet Mn$_{3}$Ir. The non-monotonous dependence of the damping on the magnon frequency makes the large momentum excitations attractive in the terahertz spintronics. To this end, we analyze the real-time and real-space dynamics of the magnetic modes, including their strongly chirality-dependent attenuation.
We present first principles charge- and spin-selfconsistent electronic structure computations on the Heusler-type disordered alloys Fe$_{3-x}$V$_{x}$X for three different metalloids X=(Si, Ga and Al). In these calculations we use the methodology based on the Korringa-Kohn- Rostoker formalism and the coherent-potential approximation (KKR-CPA), generalized to treat disorder in multi-component complex alloys.
Magnetic properties of a $σ-$Fe$_{16}$Cr$_{14}$ alloy calculated with the charge and spin self- consistent Korringa-Kohn-Rostoker (KKR) and combined with coherent potential approximation (KKR-CPA) methods are reported. Non-magnetic state as well as various magnetic orderings were considered, i.e. ferromagnetic (FM) and more complex anti-parallel (called APM) arrangements for selected sublattices, as follows from the symmetry analysis. It has been shown that the Stoner criterion applied to non-magnetic density of states at the Fermi energy, $E_F$ is satisfied for Fe atoms situated on all five l…
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…
Electronic structure calculations, using the charge and spin self-consistent Korringa- Kohn-Rostoker (KKR) method, have been performed for several $R$Mn$X$ compounds ($R$ = Mg, Ca, Sr, Ba, Y; $X$ = Si, Ge) of the CeFeSi-type structure. The origin of their magnetic properties has been investigated emphasizing the role of the Mn sublattice. The significant influence of the Mn-Mn and Mn-$X$ interatomic distances on the Mn magnetic moment value is delineated from our computations, supporting many neutron diffraction data. We show that the marked change of $μ_{Mn}$ with the Mn-Mn and Mn-$X$ distanc…
The electronic, magnetic and transport properties of Fe intercalated 2H-TaS$_2$ have been investigated by means of the Korringa-Kohn-Rostoker (KKR) method. The non-stoichiometry and disorder in the system has been accounted for using the Coherent Potential Approximation (CPA) alloy theory. A pronounced influence of disorder on the spin magnetic moment has been found for the ferro-magnetically ordered material. The same applies for the spin-orbit induced orbital magnetic moment and magneto-crystalline anisotropy energy. The temperature-dependence of the resistivity of disordered 2H-Fe$_{0.28}$T…
The Korringa-Kohn-Rostoker Green (KKR) function method for non-collinear magnetic structures was applied on Mn and Cr ad-clusters deposited on the Ni(111) surface. By considering various dimers, trimers and tetramers, a large amount of collinear and non-collinear magnetic structures is obtained. Typically all compact clusters have very small total moments, while the more open structures exhibit sizeable total moments, which is a result of the complex frustration mechanism in these systems. Thus, as the motion of a single adatom changes the cluster structure from compact to open and vice versa,…
Magnetic nanostructures on non-magnetic or magnetic substrates have attracted strong attention due to the development of new experimental methods with atomic resolution. Motivated by this progress we have extended the full-potential Korringa-Kohn-Rostoker (KKR) Green function method to treat non-collinear magnetic nanostructures on surfaces. We focus on magnetic 3d impurity nanoclusters, sitting as adatoms on or in the first surface layer on Ni(001), and investigate the size and orientation of the local moments and moreover the stabilization of non-collinear magnetic solutions. While clusters …
The modification of the magnetization dissipation or Gilbert damping caused by an inhomogeneous magnetic structure and expressed in terms of a wave vector dependent tensor $\underlineα(\vec{q})$ is investigated by means of linear response theory. A corresponding expression for $\underlineα(\vec{q})$ in terms of the electronic Green function has been developed giving in particular the leading contributions to the Gilbert damping linear and quadratic in $q$. Numerical results for realistic systems are presented that have been obtained by implementing the scheme within the framework of the fully …
Dispersion and lifetimes of magnons in non-collinear magnets from time dependent density functional theory
Institute for Theoretical Physics, Johannes Kepler University（约翰内斯·开普勒大学理论物理研究所）；Hamburg University of Applied Sciences（汉堡应用科学大学）；Max Planck Institute of Microstructure Physics（马克斯·普朗克微观结构物理研究所）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）
We introduce the Korringa-Kohn-Rostocker non-local coherent potential approximation (KKR-NLCPA) for describing the electronic structure of disordered systems. The KKR-NLCPA systematically provides a hierarchy of improvements upon the widely used KKR-CPA approach and includes non-local correlations in the disorder configurations by means of a self-consistently embedded cluster. The KKR-NLCPA method satisfies all of the requirements for a successful cluster generalization of the KKR-CPA; it remains fully causal, becomes exact in the limit of large cluster sizes, reduces to the KKR-CPA for a sing…
Electric polarization driven by non-collinear spin alignment investigated by first principles calculations
Institute of Materials Science, TU Darmstadt（达姆施塔特工业大学材料科学研究所）；Department of Chemistry/Phys. Chemistry, LMU Munich（慕尼黑大学化学/物理化学系）；New Technologies Research Center, University of West Bohemia（西波希米亚大学新技术研究中心）
The electronic and magnetic bulk properties of half-metallic Heusler alloys such as Co$_{2}$FeSi, Co$_{2}$FeAl, Co$_{2}$MnSi and Co$_{2}$MnAl are investigated by means of {\em ab initio} calculations in combination with Monte Carlo simulations. The electronic structure is analyzed using the plane wave code Quantum Espresso and magnetic exchange interactions are determined using the KKR method. From the magnetic exchange interactions the Curie temperature is obtained via Monte Carlo simulations. In addition, electronic transport properties of the trilayer systems consisting of two semi-infinite…
An analysis of the magnetocaloric properties of the pure and substituted Fe2P compounds is made based on KKR-CPA electronic structure calculations and magnetisation M(H,T) measurements. The computed electronic densities of states and magnetic moments are used to calculate both the values of the electronic and magnetic entropies, which fairly agree with the experimental findings. To enlighten the magnetic properties above Curie temperature, the paramagnetic state behaviours are simulated using the disordered local moments (DLM) concept. The KKR-CPA computations show, that in Fe2P, the Fe magnet…
An important contribution to the thermoelectric and spin-caloric transport properties in magnetic materials at elevated temperatures is the formation of a spin-disordered state due to local moment fluctuations. This effect has not been largely investigated so far. We focus on various magnetic nanostructures of CrTe in the form of thin layers or nanowires embedded in ZnTe matrix, motivated by the miniaturization of spintronics devices and by recent suggestions that magnetic nanostructures can lead to extraordinary thermoelectric effects due to quantum confinement. The electronic structure of th…
We propose a framework for optimization of the chemical composition of multinary compounds with the aid of machine learning. The scheme is based on first-principles calculation using the Korringa-Kohn-Rostoker method and the coherent potential approximation (KKR-CPA). We introduce a method for integrating datasets to reduce systematic errors in a dataset, where the data are corrected using a smaller and more accurate dataset. We apply this method to values of the formation energy calculated by KKR-CPA for nonstoichiometric systems to improve them using a small dataset for stoichiometric system…
In this Comment, using Korringa-Kohn-Rostoker coherent-potential approximation method in the atomic-sphere approximation (KKR-ASA CPA) to describe the effects of disorder due to excess Fe in FeTe alloys, we show that (i) the rigid-band approximation is inadequate to describe the effects of disorder and its application leads to an incorrect description of the underlying physics, (ii) the rigid-band energy shift of ~0.76 eV for going from FeTe to Fe_{1.068}Te (or Fe_{1.063}Te), as obtained by Han and Savrasov (Phys. Rev. Lett. 103, 067001(2009)), is inconsistent with our FP-LMTO as well as the K…
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…
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…
The anomalous Hall effect (AHE) is a well-known fundamental property of ferromagnetic metals, commonly associated with the presence of a net magnetization. Recently, an AHE has been discovered in non-collinear antiferromagnetic (AFM) metals. Driven by non-vanishing Berry curvature of AFM materials with certain magnetic space group symmetry, anomalous Hall conductivity (AHC) is very sensitive to the specific type of magnetic ordering. Here, we investigate the appearance of AHC in antiperovskite GaNMn$_{3}$ as a representative of broader materials family ANMn$_{3}$ (A is a main group element), w…
We investigate the spin-orbit torque exerted on the magnetic moments of the transition-metal impurities Cr, Mn, Fe and Co, embedded in the surface of the topological insulator Bi$_{2}$Te$ _{3} $, in response to an electric field and a consequent electrical current flow in the surface. The multiple scattering problem of electrons off impurity atoms is solved by first-principles calculations within the full-potential relativistic Korringa-Kohn-Rostoker (KKR) Green function method, while the spin-orbit torque calculations are carried out by combining the KKR method with the semiclassical Boltzman…
We present a thorough theoretical assessment of the stability of non-collinear spin arrangements in small palladium clusters. We generally find that ferromagnetic order is always preferred, but that antiferromagnetic and non-collinear configurations of different sorts exist and compete for the first excited isomers. We also show that the ground state is insensitive to the choice of atomic configuration for the pseudopotential used and to the approximation taken for the exchange and correlation potential. Moreover, the existence and relative stability of the different excited configurations als…
We show that in magnetic nanostructures with a homogeneous magnetic order, the equilibrium spin current can be nonzero. For example, this is the case of a wide magnetic ring with the magnetization along the ring axis. The physical reason of this effect is a variation of the orientation of anisotropy axis inducing a spin torque acting on the magnetic ions. The mechanism of the spin current generation is related to the quantum vacuum fluctuations in the magnetic system.
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…
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, …
ASE2SPRKKR: a unified Python framework integrating the Spin-Polarized Relativistic Korringa-Kohn-Rostoker method into the Atomic Simulation Environment
University of West Bohemia in Pilsen（比尔森西波希米亚大学）；FZU – Institute of Physics, Czech Academy of Sciences, v.v.i（捷克科学院物理研究所）；Ludwig-Maximilians-Universität München（慕尼黑路德维希-马克西米利安大学）
Spintronic applications, which rely on spin torques for operation, would greatly benefit from a non-collinear alignment between magnetizations of adjacent ferromagnetic layers for maximum performance and reliability. We demonstrate that such an alignment can be created and controlled by coupling two ferromagnetic layers across magnetic coupling layers. These coupling layers consist of a non-magnetic material, Ru, alloyed with ferromagnetic elements of Co or Fe. Changing the composition and thickness of the coupling layer enables control of the relative angle between the magnetizations of ferro…
Magnetic annealing of the collinear antiferromagnet PdMn with excess Pd produces strongly pinned magnetic moments in the annealing field direction. This behaviour can be understood with the help of the magnetic-field-biased diffusion model. Here, the magnetic field creates an energy difference between the two possible occupations of the antiferromagnetic Mn-sublattices by the Pd-excess atoms. This, mediated by diffusion, leads to an imbalance in the amount of the Pd-excess atoms in these sublattices and, subsequently, to an imbalance in the total magnetization of the sublattices. We investigat…
We predict a large anomalous Nernst effect in the inverse Heusler compensated ferrimagnets Ti$_2$Mn$X$ ($X$=Al,Ga,In) with vanishing net magnetic moments. Though the net magnetic moment is zero, the Weyl points in these systems lead to a large anomalous Nernst conductivity (ANC) due to the lack of a magnetic sublattice that inverses the sign of the Berry curvature. In comparison to the noncollinear antiferromagnets Mn$_3$Sn and Mn$_3$Ge, the high ANC stems almost entirely from the Weyl points in this class of compounds, and thus, it is topologically protected. This work shows for the first tim…
Results of the first principles study on the electronic structure and magnetism of the superconducting weak ferromagnet Y$_4$Co$_3$, are presented. Using the full potential Korringa-Kohn-Rostoker (FP-KKR) method, densities of states, dispersion curves and magnetic moments were calculated for quasi-ordered structural model of the compound in the framework of the local density approximation. Spin-polarized KKR calculations confirm that weak ferromagnetic properties of Y$_4$Co$_3$ can be attributed to only one cobalt atom located on (2b) site in the unit cell, while other twenty Co and Y atoms ac…
Previous studies on the anomalous Hall effect in coplanar non-collinear antiferromagnets are revisited and extended to magneto-optic properties, namely magneto-optic Kerr effect (MOKE) and X-ray magnetic dichroism (XMCD). Starting from group-theoretical considerations the shape of the frequency-dependent conductivity tensor for various actual and hypothetical spin configurations in cubic and hexagonal Mn$_3X$ compounds is determined. Calculated MOKE and X-ray dichroism spectra are used to confirm these findings and to give estimates of the size of the effects. For Mn$_3$IrPt and Mn$_3$PtRh all…
Electric susceptibility of antiferromagnetic multiferroics with cycloidal spin order at magnetoelectric effect associated with collinear component of spins
Ferrimagnets containing several partially compensated magnetic sublattices are considered the most promising materials for all-optical data storage and for ultrafast communications based on spin waves. There are two magnetic phases of the ferrimagnets: collinear and non-collinear ones. Up to now spin dynamics in ferrimagnets has been studied mostly in the collinear state without paying much attention to the kind of the magnetic phase. Here we investigate laser induced ultrafast spin dynamics in a rare-earth iron garnet film in the noncollinear phase as well. We identify a crucial influence of …
The influence of the spin-orbit coupling on the magnetic structure of deposited transition metal nanostructure systems has been studied by fully relativistic electronic structure calculations. The interplay of exchange coupling and magnetic anisotropy was monitored by studying the corresponding magnetic torque calculated within ab-initio and model approaches. It is found that a spin-orbit induced Dzyaloshinski-Moriya interaction can stabilise a non-collinear spin structure even if there is a pronounced isotropic ferromagnetic exchange interaction between the magnetic atoms.
Mn5Ge3 thin films epitaxially grown on Ge(111) exhibit metallic conductivity and strong ferromagnetism up to about 300 K. Recent experiments suggest a non-collinear spin structure. In order to gain deep insights into the magnetic structure of this compound, we have performed fully unconstrained ab-initio pseudopotential calculations within density functional theory, investigating the different magnetic states corresponding to Collinear (C) and Non-Collinear (NC) spin configurations. We focus on their relative stability under pressure and strain field. Under pressure, the C and NC configuration…
Spin rectification in a single crystal Fe/Au/Fe sandwich is electrically detected for collinear and non-collinear magnetization and external magnetic field configurations. The line shape, line width and signal polarity are analysed. The spin rectication theory has been much extended by taking the magneto-crystalline anisotropy and shape anisotropy into account, which explained non-collinear resonances and agrees very well with experimental data. Thus, a comprehensive understanding of spin rectification in ferromagnetic metal was demonstrated in this work.
Anomalous magnetotransport in a non-collinear correlated kagome ferromagnet MgMn6Sn6
S. N. Bose National Centre for Basic Sciences（S.N. 玻色基础科学国家中心）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；ISIS Neutron and Muon Source, Science and Technology Facilities Council, Rutherford Appleton Laboratory（ISIS中子与μ子源，科学与技术设施委员会，拉瑟福德阿普尔顿实验室）；School of Physical Sciences, Indian Institute of Technology Goa（印度果阿理工学院物理科学学院）
By means of ab initio calculations based on the density functional theory we investigated magnetic phase diagram of ordered FePd$_3$ alloy as a function of external pressure. Considering several magnetic configurations we concluded that the system under pressure has a tendency to non-collinear spin alignment. Analysis of the Heisenberg exchange parameters $J_{ij}$ revealed strong dependence of iron-iron magnetic couplings on polarization of Pd atoms. To take into account the latter effect we built an extended Heisenberg model with higher order (biquadratic) terms. Minimizing the energy of this…
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…
The magnetic force theorem provides convenient ways to study exchange interactions in magnetic systems. However, it is well known that short range interactions in itinerant magnetic systems are poorly described with the conventional use of the theorem and numerous strategies have been developed over the years to overcome this deficiency. In this study, we discuss this issue in the context of the frozen magnon method and find that a self-consistent approach is in general preferable. Moreover, an extended Heisenberg model is suggested in order to better describe finite deviations from the magnet…
We report the observation of a large anisotropic topological Hall effect (THE) in the hexagonal non-collinear magnet Fe5Sn3 single crystals. It is found that the sign of the topological Hall resistivity is negative when a magnetic field H perpendicular to the bc-plane (H\perp bc-plane), however, it changes form negative to positive when H parallel to the c-axis (H\parallel c-axis). The value of topological Hall resistivity increased with the increasing temperature and reached approximately -2.12 μΩcm (H\perp bc-plane) and 0.5 μΩcm (H\parallel c-axis) at 350 K, respectively. Quantitative analys…
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）
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…
The low-temperature magnetic structure of \HG has been studied by high-resolution powder neutron diffraction. Long-range incommensurate magnetic order sets in at T$_N\sim$22K with propagation vector \textbf{k}=(0,0,$\sim$0.18). On cooling below T$_N$, the propagation vector increases and saturates at the commensurate value \textbf{k}=(0,0,0.25). The magnetic structure below T$_N$ consists of ferromagnetic layers in the \textit{ab}-plane stacked in a spiral arrangement along the \textit{c}-axis. Symmetry analysis using corepresentations theory reveals a point group symmetry in the ordered magne…
