arXiv subjects

I. V. Solovyev

Publications and source records attributed to I. V. Solovyev.

At least 37 records · Page 2Linked to original sources

arXiv2016

Pressure dependence of the structure and electronic properties of Sr3Ir2O7

We study the structural evolution of Sr$_3$Ir$_2$O$_7$ as a function of pressure using x-ray diffraction. At a pressure of 54 GPa at room temperature, we observe a first-order structural phase transition, associated with a change from tetragonal to monoclinic symmetry, and accompanied by a 4% volume collapse. Rietveld refinement of the high-pressure phase reveals a novel modification of the Ruddlesden-Popper structure, which adopts an altered stacking sequence of the perovskite bilayers. As the positions of the oxygen atoms could not be reliably refined from the data, we use density functional theory (local-density approximation+$U$+spin orbit) to optimize the crystal structure, and to elucidate the electronic and magnetic properties of Sr$_3$Ir$_2$O$_7$ at high pressure. In the low-pressure tetragonal phase, we find that the in-plane rotation of the IrO$_6$ octahedra increases with pressure. The calculations further indicate that a bandwidth-driven insulator-metal transition occurs at $\sim$20 GPa, along with a quenching of the magnetic moment. In the high-pressure monoclinic phase, structural optimization resulted in complex tilting and rotation of the oxygen octahedra, and strongly overlapping $t_{2g}$ and $e_g$ bands. The $t_{2g}$ bandwidth renders both the spin-orbit coupling and electronic correlations ineffectual in opening an electronic gap, resulting in a robust metallic state for the high-pressure phase of Sr$_3$Ir$_2$O$_7$.

cond-mat.str-el↗

arXiv2016

Hybridization and spin-orbit coupling effects in quasi-one-dimensional spin-1/2 magnet Ba3Cu3Sc4O12

We study electronic and magnetic properties of the quasi-one-dimensional spin-1/2 magnet Ba3Cu3Sc4O12 with a distinct orthogonal connectivity of CuO4 plaquettes. An effective low-energy model taking into account spin-orbit coupling was constructed by means of first-principles calculations. On this basis a complete microscopic magnetic model of Ba3Cu3Sc4O12, including symmetric and antisymmetric anisotropic exchange interactions, is derived. The anisotropic exchanges are obtained from a distinct first-principles numerical scheme combining, on one hand, the local density approximation taking into account spin-orbit coupling, and, on the other hand, projection procedure along with the microscopic theory by Toru Moriya. The resulting tensors of the symmetric anisotropy favor collinear magnetic order along the structural chains with the leading ferromagnetic coupling J1 = -9.88 meV. The interchain interactions J8 = 0.21 meV and J5 = 0.093 meV are antiferromagnetic. Quantum Monte Carlo simulations demonstrated that the proposed model reproduces the experimental Neel temperature, magnetization and magnetic susceptibility data. The modeling of neutron diffraction data reveals an important role of the covalent Cu-O bonding in Ba3Cu3Sc4O12.

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arXiv2016

Band filling dependence of the Curie temperature in CrO2

Rutile CrO$_2$ is an important half-metallic ferromagnetic material, which is also widely used in magnetic recording. In an attempt to find the conditions, which lead to the increase the Curie temperature ($T_{\rm C}$), we study theoretically the band-filling dependence of interatomic exchange interactions in the rutile compounds. For these purposes, we use the effective low-energy model for the magnetic $t_{2g}$ bands, derived from the first-principles electronic structure calculations in the Wannier basis, which is solved by means of dynamical mean-field theory. After the solution, we calculate the interatomic exchange interactions, by using the theory of infinitesimal spin rotations, and evaluate $T_{\rm C}$. We argue that, as far as the Curie temperature is concerned, the band filling realized in CrO$_2$ is far from being the optimal one and much higher $T_{\rm C}$ can be obtained by decreasing the number of $t_{2g}$ electrons ($n$) via the hole doping. We find that the optimal $n$ is close to $1$, which should correspond to the case of VO$_2$, provided that it is crystallized in the rutile structure. This finding was confirmed by using the experimental rutile structure for both CrO$_2$ and VO$_2$ and reflects the general tendency towards ferromagnetism for the narrow-band compounds at the beginning of the band filling. In particular, our results suggest that the strong ferromagnetism can be achieved in the thin films of VO$_2$, whose crystal structure is controlled by the substrate.

cond-mat.str-el↗

arXiv2015

Validity and limitations of the superexchange model for the magnetic properties of Sr2IrO4 and Ba2IrO4 mediated by the strong spin-orbit coupling

Layered perovskites Sr2IrO4 and Ba2IrO4 are regarded as the key materials for understanding the properties of magnetic relativistic insulators, mediated by the strong spin-orbit (SO) coupling. One of the most fundamental issues is to which extent these properties can be described by the superexchange (SE) model, formulated in the limit of the large Coulomb repulsion. In the present work we address this issue by deriving the relevant models and extracting parameters of these models from the first-principles calculations. First, we construct the effective Hubbard-type model for the t2g bands, by recasting the problem in the language of Wannier orbitals. Then, we map the obtained electron model onto the pseudospin model by applying the theory of SE interactions. We discuss the microscopic origin of anisotropic SE interactions, inherent to the compass Heisenberg model, and the appearance of the antisymmetric Dzyaloshinskii-Moriya term, associated with the additional rotation of the IrO6 octahedra in Sr2IrO4. In order to evaluate the Neel temperature (TN), we employ the non-linear sigma model. While for Sr2IrO4 our value of TN agrees with the experimental one, for Ba2IrO4 it is overestimated by a factor two. We argue that this discrepancy is related to limitations of the SE model: while for more localized t2g states in Sr2IrO4 it works reasonably well, the higher-order terms, beyond the SE model, play a more important role in the more "itinerant" Ba2IrO4, giving rise to the new type of isotropic and anisotropic exchange interactions. This conclusion is supported by unrestricted Hartree-Fock calculations for the same electron model, where in the case of Ba2IrO4, already on the mean-field level, we were able to reproduce the experimentally observed magnetic ground state, while for Sr2IrO4 the main results are essentially the same as in the SE model.

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arXiv2015

Mechanisms and origins of half-metallic ferromagnetism in CrO2

Chromium dioxide (CrO2) offers a rare example of metallic ferromagnetism among stoichiometric transition-metal oxides. What makes it even more remarkable is the half-metallic electronic structure. Today, CrO2 is widely used in magnetorecording and regarded as a promising spintronic material. Nevertheless, the key question "Why is it ferromagnetic?" remains largely unanswered, despite general interest to the problem and practical importance of CrO2. In the present work we challenge this question by combining first-principles electronic structure calculations with the model Hamiltonian approach and modern many-body methods for treating electron correlations. Our analysis demonstrates that the problem is indeed highly nontrivial: at the first glance, the ferromagnetism in CrO2 can be easily explained by Hund's rule related exchange processes in the narrow t2g band. However, the electron correlations, rigorously treated in the frameworks of dynamical mean-field theory, tend to destabilize this state. The ferromagnetism reemerges if, besides conventional kinetic energy changes in the t2g band, to consider other mechanism, involving direct exchange and magnetic polarization of the oxygen band. We show how all these contributions can be evaluated using first-principles electronic structure calculations. Our results explain the overall stability of the ferromagnetic state and provide the firm microscopic basis for understanding the magnetism of CrO2.

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arXiv2015

Microscopic analysis of the magnetic form factor in low-dimensional cuprates

We analyze the magnetic form factor of Cu$^{2+}$ in low-dimensional quantum magnets by taking the metal-ligand hybridization into account explicitly. In this analysis we use the form of magnetic Wannier orbitals, derived from the first-principles calculations, and identify the contributions of different atomic sites. Having performed local density approximation calculations for cuprates with different types of ligand atoms, we discuss the influence of the on-site Coulomb correlations on the structure of the magnetic orbital. The typical composition of Wannier functions for copper oxides, chlorides and bromides is defined and related to features of the magnetic form factor. We propose easy-to-use approximations of the partial orbital contributions to the magnetic form factor in order to give a microscopic explanation for the results obtained in previous first-principles studies.

cond-mat.str-el↗

arXiv2015

Magnetization induced local electric dipoles and multiferroic properties of Ba2CoGe2O7

Ba2CoGe2O7, crystallizing in the noncentrosymmetric but nonpolar structure, belongs to a special class of multiferroic materials, whose properties are predetermined by the rotoinversion symmetry. Unlike inversion, the rotoinversion symmetry can be easily destroyed by the magnetization. Moreover, due to specific structural pattern, the magnetic structure of Ba2CoGe2O7 is relatively soft. Altogether, this leads to the rich variety of multiferroic properties, where the magnetic structure can be easily deformed by the magnetic field, inducing the electric polarization in the direction, which depends on the direction of the magnetic field. In this paper, we show that all these properties can be successfully explained on the basis of realistic low-energy model, derived from the first-principles electronic structure calculations for the magnetically active Co 3d bands, and the Berry-phase theory of electric polarization. Particularly, we argue that the magnetization induced electric polarization in Ba2CoGe2O7 is essentially local and expressed via the expectation values of some dipole matrices, calculated in the Wannier basis of the model, and the site-diagonal density matrices of the magnetic Co sites. Thus, the basic aspects of the behavior of Ba2CoGe2O7 can be understood already in the atomic limit, where both magnetic anisotropy and magnetoelectric coupling are specified by density matrix. Then, the macroscopic polarization can be found as a superposition of electric dipoles of the individual Co sites. We discuss the behavior of interatomic magnetic interactions, main contributions to the magnetocrystalline anisotropy and the spin canting, as well as the similarities and differences of the proposed picture from the phenomenological model of spin-dependent p-d hybridization.

cond-mat.mtrl-sci↗

arXiv2014

First principles investigation of exchange interactions in quasi-one-dimensional antiferromagnet CaV2O4

The effect of orbital degrees of freedom on the exchange interactions in the spin-1 quasi-one-dimensional antiferromagnet CaV2O4 is systematically studied. For this purpose a realistic low-energy model with the parameters derived from the first-principles calculations is constructed. The exchange interactions are calculated using both the theory of infinitesimal spin rotations near the mean-field ground state and the superexchange model, which provide a consistent description. The obtained behaviour of exchange interactions substantially differs from the previously proposed phenomenological picture based on the magnetic measurements and structural considerations, namely: (i) Despite quasi-one-dimensional character of the crystal structure, consisting of the zigzag chains of edge-sharing VO6 octahedra, the electronic structure is essentially three-dimensional, that leads to finite interactions between the chains; (ii) The exchange interactions along the legs of the chains appear to dominate; and (iii) There is a substantial difference of exchange interactions in two crystallographically inequivalent chains. The combination of these three factors successfully reproduces the behaviour of experimental magnetic susceptibility.

cond-mat.mtrl-sci↗

arXiv2014

Spin dependence of ferroelectric polarization in the double exchange model for manganites

The double exchange (DE) model is systematically applied for studying the coupling between ferroelectric (FE) and magnetic orders in several prototypical types of multiferroic manganites. The model was constructed for the magnetically active Mn $3d$ bands in the basis of Wannier functions and include the effect of screened on-site Coulomb interactions. The essence of our approach for the FE polarization is to use the Berry phase theory, formulated in terms of occupied Wannier functions, and to evaluate the asymmetric spin-dependent change of these functions in the framework of the DE model. This enables us to quantify the effect of the magnetic symmetry breaking and derive several useful expressions for the electronic polarization ${\bf P}$, depending on the relative directions of spins. The proposed theory is applied to the solution of three major problems: (i) The magnetic-state dependence of ${\bf P}$ in hexagonal manganites; (ii) The microscopic relationship between canted ferromagnetism and ${\bf P}$ in monoclinic BiMnO$_3$; (iii) The origin of FE activity in orthorhombic manganites. We show that for an arbitrary noncollinear magnetic structure, propagating along the orthorhombic $\boldsymbol{b}$ axis and antiferromagnetically coupled $\boldsymbol{c}$, ${\bf P}$ can be obtained by scaling the one of the E-phase with the prefactor depending only on the relative directions of spins and being the measure of the spin inhomogeneity. This picture works equally well for the twofold (HoMnO$_3$) and fourfold (TbMnO$_3$) periodic manganites. The basic difference is that the twofold periodic magnetic structure is strongly inhomogeneous, that leads to large ${\bf P}$. On the contrary, the fourfold periodic magnetic structure can be viewed as a moderately distorted homogeneous spin spiral, which corresponds to weaker ${\bf P}$.

cond-mat.str-el↗

arXiv2014

Self-consistent linear response for the spin-orbit interaction related properties

In many cases, the relativistic spin-orbit (SO) interaction is regarded to be small and can be treated using perturbation theory. The major obstacle on this route comes from the fact that the SO interaction can also polarize the electron system and produce additional contributions to the perturbation theory, arising from the electron-electron interactions. In electronic structure calculations, it may even lead to necessity to abandon the perturbation theory and return to the self-consistently solution of Kohn-Sham-like equations with the effective potential $\hat{v}$, incorporating the effects of the electron-electron interactions and the SO coupling, even though the latter is small. In this work, we present the theory of self-consistent linear response (SCLR), which allows us to get rid of numerical self-consistency and formulate it analytically in the first order of the SO coupling. This strategy is applied to the Hartree-Fock solution of the effective Hubbard model, derived from electronic structure calculations in the Wannier basis. By using $\hat{v}$, obtained from SCLR, one can successfully reproduce results of ordinary calculations for the orbital magnetization and other properties in the first order of the SO coupling. Particularly, SCLR appears to be extremely useful for calculations of antisymmetric Dzyaloshinskii-Moriya (DM) interactions based on the magnetic force theorem. Furthermore, due to the powerful 2n+1 theorem, the SCLR theory allows us to calculate the magnetic anisotropy energy up to the third order of the SO coupling. The fruitfulness of this approach is illustrated on a number of example, including the spin canting in YTiO$_3$ and LaMnO$_3$, formation of spiral magnetic order in BiFeO$_3$, and the magnetic inversion symmetry breaking in BiMnO$_3$, which gives rise to both ferroelectric activity and DM interactions, responsible for the ferromagnetism.

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arXiv2013

Orbital magnetization of insulating perovskite transition-metal oxides with the net ferromagnetic moment in the ground state

Modern theory of the orbital magnetization is applied to the series of insulating perovskite transition metal oxides (orthorhombic YTiO$_3$, LaMnO$_3$, and YVO$_3$, as well as monoclinic YVO$_3$), carrying a net ferromagnetic (FM) moment in the ground state. For these purposes, we use an effective Hubbard-type model, derived from the first-principles electronic-structure calculations and describing the behavior of magnetically active states near the Fermi level. The solution of this model in the mean-field Hartree-Fock approximation with the relativistic spin-orbit coupling typically gives us a distribution of the local orbital magnetic moments, which are related to the site-diagonal part of the density matrix $\hat{\cal D}$ by the "standard" expression $\boldsymbolμ^0 = - μ_{\rm B} \mathrm{Tr} \{ \hat{\textbf{L}} \hat{\cal D} \}$ and which are usually well quenched by the crystal field. In this work, we evaluate "itinerant" corrections $Δ\boldsymbol{\cal M}$ to the net FM moment, suggested by the modern theory. We show that these corrections are small and in most cases can be neglected. Nevertheless, the most interesting aspect of our analysis is that, even for these compounds, which are typically regarded as normal Mott insulators, the "itinerant" corrections reveal a strong $\textbf{k}$-dependence in the reciprocal space, following the behavior of Chern invariants. Therefore, the small value of $Δ\boldsymbol{\cal M}$ is the result of strong cancelation of relatively large contributions, coming from different parts of the Brillouin zone. We discuss details as well as possible implications of this cancelation, which depends on the crystal structure as well as the type of the magnetic ground state.

cond-mat.mtrl-sci↗

arXiv2013

Magnetism of sodium superoxide

By combining first-principles electronic-structure calculations with the model Hamiltonian approach, we systematically study the magnetic properties of sodium superoxide (NaO2), originating from interacting superoxide molecules. We show that NaO2 exhibits a rich variety of magnetic properties, which are controlled by relative alignment of the superoxide molecules as well as the state of partially filled antibonding molecular π_g-orbitals. The orbital degeneracy and disorder in the high-temperature pyrite phase gives rise to weak isotropic antiferromagnetic (AFM) interactions between the molecules. The transition to the low-temperature marcasite phase lifts the degeneracy, leading to the orbital order and formation of the quasi-one-dimensional AFM spin chains. Both tendencies are consistent with the behavior of experimental magnetic susceptibility data. Furthermore, we evaluate the magnetic transition temperature and type of the long-range magnetic order in the marcasite phase. We argue that this magnetic order depends on the behavior of weak isotropic as well as anisotropic and Dzyaloshinskii-Moriya exchange interactions between the molecules. Finally, we predict the existence of a multiferroic phase, where the inversion symmetry is broken by the long-range magnetic order, giving rise to substantial ferroelectric polarization.

cond-mat.mtrl-sci↗

arXiv2013

Double-exchange theory of ferroelectric polarization in orthorhombic manganites with twofold periodic magnetic texture

We argue that many aspects of improper ferroelectric activity in orthorhombic manganites can be rationalized by considering the limit of infinite intra-atomic splitting between the majority- and minority-spin states (or the double exchange limit), which reduces the problem to the analysis of a spinless double exchange (DE) Hamiltonian. We apply this strategy to the low-energy model, derived from the first-principles calculations, and combine it with the Berry-phase theory of electric polarization. We start with the simplest two-orbital model, describing the behavior of the eg bands, and apply it to the E-type antiferromagnetic (AFM) phase, which in the DE limit effectively breaks up into one-dimensional zigzag chains. We derive an analytical expression for the electronic polarization (Pel) and explain how it depends on the orbital ordering and the energy splitting Delta between eg states. Then, we evaluate parameters of this model, starting from a more general five-orbital model for all Mn 3d bands and constructing a new downfolded model for the eg bands. From the analysis of these parameters, we conclude that the behavior of Pel in realistic manganites corresponds to the limit of large Delta. We further utilize this property in order to derive an analytical expression for Pel in a general two-fold periodic magnetic texture, based on the five-orbital model and the perturbation-theory expansion for the Wannier functions in the first order of 1/Delta. This expression explains the functional dependence of Pel on the relative directions of spins. Furthermore, it suggests that Pel is related to the asymmetry of the transfer integrals, which should simultaneously have symmetric and antisymmetric components. Finally, we explain how the polarization can be switched between orthorhombic directions a and c by inverting the zigzag AFM texture in every second ab plane.

cond-mat.str-el↗

arXiv2012

Origin of Multiferroicity in MnWO4

MnWO4 is regarded as a canonical example of multiferroic materials, where the multiferroic activity is caused by a spin-spiral alignment. We argue that, in reality, MnWO4 has two sources of the spin-spirality, which conflict with each other. One is the Dzyaloshinskii-Moriya (DM) interactions, reflecting the P2/c symmetry of the lattice. The P2/c structure of MnWO4 has an inversion center, that connects two Mn sublattices. Therefore, from the viewpoint of DM interactions, different Mn sublattices are expected to have opposite spin chirality. Another source is competing isotropic exchange interactions, which tend to form a spin-spiral texture with the same chirality in both magnetic sublattices. Thus, there is a conflict between DM and isotropic exchange interactions, which makes these two sublattices inequivalent and, therefore, breaks the inversion symmetry. Our theoretical analysis is based on the low-energy model, derived from the first-principles electronic structure calculations.

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arXiv2012

Mn$_2$FeSbO$_6$: a ferrimagnetic ilmenite and an antiferromagnetic perovskite

Due of its polymorphism, Mn$_2$FeSbO$_6$ can be synthesized at high pressures and temperatures as a ferrimagnetic ilmenite or an antiferromagnetic perovskite. The structural phase transformation is discussed in detail, and magnetic structures are proposed for both phases. The high-pressure Mn$_2$FeSbO$_6$ polymorph is a rare example of $A_2 B'B"$O$_6$ perovskite with solely Mn cations on the $A$-site. Fe and Sb cations are ordered on the $B$-sites. Theoretical calculations for the perovskite phase suggest a complex magnetic structure, holding an electronic polarization.

cond-mat.str-el↗

arXiv2012

Magnetic structure and ferroelectric activity in orthorhombic YMnO3: relative roles of magnetic symmetry breaking and atomic displacements

We discuss relative roles played by the magnetic inversion symmetry breaking and the ferroelectric (FE) atomic displacements in the multiferroic state of YMnO3. For these purposes we derive a realistic low-energy model, using results of first-principles calculations and experimental parameters of the crystal structure. Then, we solve this model in the Hartree-Fock approximation. We argue that the multiferroic state in YMnO3 has a magnetic origin, and the centrosymmetric Pbnm structure is formally sufficient for explaining details of the noncentrosymmetric magnetic ground state. The relativistic spin-orbit interaction lifts the degeneracy, caused by the frustration of isotropic interactions, and stabilizes a twofold periodic magnetic state, which is similar to the E-state apart from the spin canting. The noncentrosymmetric atomic displacements in the P2_1nm phase reduce the spin canting, but do not change the symmetry of the magnetic state. The effect of the P2_1nm distortion on the FE polarization P_a is twofold: (i) it gives rise to ionic contributions, associated with the Y and O sites; (ii) it affects the electronic polarization, through the change of the spin canting. The relatively small value of P_a, observed in the experiment, is caused by a partial cancelation of the electronic and ionic contributions in the experimental P2_1nm structure. Finally, we theoretically optimize the crystal structure, by using the LSDA+U approach and assuming the collinear E-type alignment. We have found that the agreement with the experimental data in this case is less satisfactory and P_a is largely overestimated. Although the magnetic structure can be formally tuned by varying the Coulomb repulsion U as a parameter, apparently LSDA+U fails to reproduce some fine details of the experimental structure, and the cancelation of different contributions in P_a does not occur.

cond-mat.mtrl-sci↗

arXiv2012

Theoretical Analysis of Electronic and Magnetic Properties of NaV$_2$O$_4$: Crucial Role of the Orbital Degrees of Freedom

Using realistic low-energy model with parameters derived from the first-principles electronic structure calculation, we address the origin of the quasi-one-dimensional behavior in orthorhombic NaV$_2$O$_4$, consisting of the double chains of edge-sharing VO$_6$ octahedra. We argue that the geometrical aspect alone does not explain the experimentally observed anisotropy of electronic and magnetic properties of NaV$_2$O$_4$. Instead, we attribute the unique behavior of NaV$_2$O$_4$ to one particular type of the orbital ordering, which respects the orthorhombic $Pnma$ symmetry. This orbital ordering acts to divide all $t_{2g}$ states into two types: the `localized' ones, which are antisymmetric with respect to the mirror reflection $y \rightarrow -$$y$, and the symmetric `delocalized' ones. Thus, NaV$_2$O$_4$ can be classified as the double exchange system. The directional orientation of symmetric orbitals, which form the metallic band, appears to be sufficient to explain both quasi-one-dimensional character of interatomic magnetic interactions and the anisotropy of electrical resistivity.

cond-mat.mtrl-sci↗

arXiv2012

Magnetic structure of hexagonal YMnO3 and LuMnO3 from a microscopic point of view

The aim of this work is to unravel a basic microscopic picture behind complex magnetic properties of hexagonal manganites. For these purposes, we consider two characteristic compounds: YMnO3 and LuMnO3, which form different magnetic structures in the ground state. First, we establish an electronic low-energy model, which describes the behavior of the Mn 3d bands of YMnO3 and LuMnO3, and derive parameters of this model from the first-principles calculations. From the solution of this model, we conclude that, despite strong frustration effects in the hexagonal lattice, the relativistic spin-orbit interactions lift the degeneracy of the magnetic ground state so that the experimentally observed magnetic structures are successfully reproduced by the low-energy model. Then, we analyze this result in terms of interatomic magnetic interactions, which were computed using different approximations (starting from the model Hamiltonian as well as directly from the first-principles electronic structure calculations in the local-spin-density approximation). We argue that the main reason why YMnO3 and LuMnO3 tend to form different magnetic structures is related to the behavior of the single-ion anisotropy, which reflects the directional dependence of the lattice distortion: namely, the expansion and contraction of the Mn-trimers, which take place in YMnO3 and LuMnO3, respectively. On the other hand, the magnetic coupling between the haxagonal planes is controlled by the next-nearest-neighbor interactions, which are less sensitive to the direction of the trimerization. Finally, using the Berry-phase formalism, we evaluate the magnetic-state dependence of the ferroelectric polarization, and discuss potential applications of the latter in magnetoelectric switching phenomena.

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