arXiv subjects

D. I. Khomskii

Publications and source records attributed to D. I. Khomskii.

At least 19 recordsLinked to original sources

arXiv2024

Evidence for distortion-induced local electric polarization in $α$-RuCl$_3$

The spin-orbit assisted Mott insulator $α$-RuCl$_3$ is a prime candidate for material realization of the Kitaev quantum spin liquid. While little attention has been paid to charge degrees of freedom, charge effects, such as electric polarization, may arise in this system. Here, we report distortion-induced local electric polarization in $α$-RuCl$_3$ as evidenced by single-crystal X-ray diffraction, second harmonic generation (SHG) and dielectric measurements. The SHG signal appears at room temperature and develops substantially in the Kitaev paramagnetic state when short-range spin correlations come into play. Despite sizable pyroelectric currents in the Kitaev paramagnetic state, the absence of hysteresis in electric field-dependent polariza-tion (P-E) points to the short-range nature of electric polarization. This localized electric polarization is likely the result of distortion-induced charge dimerization, achieved through virtual hopping-induced charge redistribution. In addition, the electric polarization is boosted by short-range spin correlations via spin-phonon coupling in the Kitaev paramagnetic state. Our results emphasize the importance of charge degrees of freedom in $α$-RuCl$_3$, which establish a novel platform to investi-gate charge effects in Kitaev materials.

cond-mat.str-el↗

arXiv2022

Magnetic oxides

In this article we give a general survey of the main properties of magnetic oxides - mostly the oxides of transition metals, but sometime also containing rare earths ions. This is a very rich class of materials, among which there are insulators and metals, systems with insulator-metal transitions, and there are among them even high-temperature superconductors. One of the main features of these compounds, which attract to them special attention and which serve as a basis of many applications, are their rich magnetic properties. In this article we discuss the main physical effects determining their behaviour, and describe in detail especially their magnetic properties, but not only. After shortly discussing the basic structure of isolated magnetic ions, we concentrate on the collective effects depending on the interaction between sites, especially exchange interaction, giving rise to different magnetic properties: different types of magnetic ordering in conventional systems, but also more exotic states such as spin liquid states in frustrated systems. We also cover related phenomena in magnetic oxides, such as magnetoelectric and multiferroic behaviour, and discuss at the end their diverse useful properties serving as a basis of many applications.

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arXiv2022

Quasimolecular electronic structure of the spin-liquid candidate Ba$_3$InIr$_2$O$_9$

The mixed-valent iridate Ba3InIr2O9 has been discussed as a promising candidate for quantum spin-liquid behavior. The compound exhibits Ir$^{4.5+}$ ions in face-sharing IrO6 octahedra forming Ir2O9 dimers with three t2g holes per dimer. Our results establish Ba3InIr2O9 as a cluster Mott insulator. Strong intra-dimer hopping delocalizes the three t2g holes in quasi-molecular dimer states while inter-dimer charge fluctuations are suppressed by Coulomb repulsion. The magnetism of Ba3InIr2O9 emerges from spin-orbit entangled quasi-molecular moments with yet unexplored interactions, opening up a new route to unconventional magnetic properties of 5d compounds. Using single-crystal x-ray diffraction we find the monoclinic space group C2/c already at room temperature. Dielectric spectroscopy shows insulating behavior. Resonant inelastic x-ray scattering (RIXS) reveals a rich excitation spectrum below 1.5 eV with a sinusoidal dynamical structure factor that unambiguously demonstrates the quasi-molecular character of the electronic states. Below 0.3 eV, we observe a series of excitations. According to exact diagonalization calculations, such low-energy excitations reflect the proximity of Ba3InIr2O9 to a hopping-induced phase transition based on the condensation of a quasi-molecular spin-orbit exciton. The dimer ground state roughly hosts two holes in a bonding j=1/2 orbital and the third hole in a bonding j=3/2 orbital.

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arXiv2022

RIXS interferometry and the role of disorder in the quantum magnet Ba$_3$Ti$_{3-x}$Ir$_{x}$O$_9$

Motivated by several claims of spin-orbit driven spin-liquid physics in hexagonal Ba$_3$Ti$_{3-x}$Ir$_x$O$_9$ hosting Ir2O9 dimers, we report on resonant inelastic x-ray scattering (RIXS) at the Ir L3 edge for different x. We demonstrate that magnetism in Ba$_3$Ti$_{3-x}$Ir$_x$O$_9$ is governed by an unconventional realization of strong disorder, where cation disorder affects the character of the local moments. RIXS interferometry, studying the RIXS intensity over a broad range of transferred momentum q, is ideally suited to assign different excitations to different Ir sites. We find pronounced Ir-Ti site mixing. Both ions are distributed over two crystallographically inequivalent sites, giving rise to a coexistence of quasimolecular singlet states on Ir2O9 dimers and spin-orbit entangled j=1/2 moments of 5d$^5$ Ir$^{4+}$ ions. RIXS reveals different kinds of strong magnetic couplings for different bonding geometries, highlighting the role of cation disorder for the suppression of long-range magnetic order in this family of compounds.

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arXiv2022

Hall Effect in Doped Mott-Hubbard Insulator

We present theoretical analysis of Hall effect in doped Mott-Hubbard insulator, considered as a prototype of cuprate superconductor. We consider the standard Hubbard model within DMFT approximation. As a typical case we consider the partially filled (hole doping) lower Hubbard band. We calculate the doping dependence of both the Hall coefficient and Hall number and determine the value of carrier concentration, where Hall effect changes its sign. We obtain a significant dependence of Hall effect parameters on temperature. Disorder effects are taken into account in a qualitative way.We also perform a comparison of our theoretical results with some known experiments on doping dependence of Hall number in the normal state of YBCO and Nd-LSCO, demonstrating rather satisfactory agreement of theory and experiment. Thus the doping dependence of Hall effect parameters obtained within Hubbard model can be considered as an alternative to a popular model of the quantum critical point.

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arXiv2022

Interplay of the Jahn--Teller Effect and Spin-Orbit Coupling: The Case of Trigonal Vibronic Modes

We study an interplay between the orbital degeneracy and spin-orbit coupling giving rise to spin-orbital entangled states. As a specific example, we analyze the interaction of electrons occupying triply degenerate single-ion $t_{2g}$ levels with trigonal vibronic modes (the $t\otimes T$ problem). A more general problem of the electron-lattice interaction involving both tetragonal and trigonal vibrations is also considered. It is shown that the result of such interaction crucially depends on the occupation of $t_{2g}$ levels leading to either the suppression or enhancement of the Jahn-Teller effect by the spin-orbit coupling.

cond-mat.mtrl-sci↗

arXiv2022

Spin-orbit coupling and crystal-field splitting in Ti-doped Ca2RuO4 studied by ellipsometry

In Ca2RuO4, the competition of spin-orbit coupling $ζ$ and tetragonal crystal field splitting $Δ_{CF}$ has been discussed controversially for many years. The orbital occupation depends on $Δ_{CF}/ζ$, which allows us to address this ratio via the optical spectral weights of the lowest intersite Mott-Hubbard excitations. We study the optical conductivity of Ca$_2$Ru$_{0.99}$Ti$_{0.01}$O$_4$ in the range of 0.75 - 5 eV by ellipsometry, using the large single crystals that can be grown for small Ti concentrations. Based on a local multiplet calculation, our analysis results in $2.4 \leq Δ_{CF}/ζ\leq 4$ at 15 K. The dominant crystal field yields a ground state close to xy orbital order but spin-orbit coupling is essential for a quantitative description of the properties. Furthermore, we observe a pronounced decrease of $Δ_{CF}$ with increasing temperature, as expected based on the reduction of octahedral distortions.

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arXiv2022

Hall effect in doped Mott insulator: DMFT-approximation

In the framework of dynamical mean field theory (DMFT) we analyze Hall effect in doped Mott insulator as a parent cuprate superconductor. We consider the partial filling (hole doping) of the lower Hubbard band and calculate the dependence of Hall coefficient and Hall number on hole doping, determining the critical concentration for sign change of the Hall coefficient. Significant temperature dependence of Hall effect is noted. A good agreement is demonstrated with concentration dependence of Hall number obtained in experiments in the normal state of YBCO.

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arXiv2022

Orbital physics: glorious past, bright future

Transition metal (TM) compounds present a very big class of materials with quite diverse properties. There are among them insulators, metals, systems with insulator-metal transitions; most magnetic systems are TM compounds; there are among them also (high-Tc) superconductors. Their very rich properties are largely determined by the strong interplay of different degrees of freedom: charge; spin; orbital; lattice. Orbital effects play a very important role in these systems -- and not only in them! The study of this field, initiated by Goodenough almost 70 years ago, turned out to be very fruitful and produced a lot of important results. In this short review I first discuss the basics of orbital physics, summarize the main achievements in this big field, in which Goodenough played a pivotal role and which are nowadays widely used to explain many properties of TM compounds. In the main part of the text I discuss novel developments and perspectives in orbital physics, which is still a very active field of research, constantly producing new surprises.

cond-mat.str-el↗

arXiv2021

Emergent 1/3 magnetization plateaus in pyroxene CoGeO$_3$

Despite the absence of an apparent triangular pattern in the crystal structure, we observe unusually well pronounced 1/3 magnetization plateaus in the quasi one-dimensional Ising spin chain compound CoGeO$_3$ which belongs to the class of pyroxene minerals. We succeeded in uncovering the detailed microscopic spin structure of the 1/3 magnetization plateau phase by means of neutron diffraction. We observed changes of the initial antiferromagnetic zero-field spin structure that are resembling a regular formation of antiferromagnetic "domain wall boundaries", resulting in a kind of modulated magnetic structure with 1/3-integer propagation vector. The net ferromagnetic moment emerges at these "domain walls" whereas two third of all antiferromagnetic chain alignments can be still preserved. We propose a microscopic model on the basis of an anisotropic frustrated square lattice to explain the observations.

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arXiv2021

Evolution of valence-specific spin states and local distortions in La$_{2-x}$Sr$_x$CoO$_4$

We present X-ray spectroscopic evidence for the evolution of valence-specific spin states and tetragonal distortions in single-layer cobaltates. Measurements of Co $L_3$-edge resonant inelastic X-ray scattering reveal the $t_{2g}$ electronic structure of Co for hole-doped La$_{2-x}$Sr$_x$CoO$_4$ ($x$ = 0.5, 0.7 and 0.8). As the Sr-doping $x$ increases, the tetragonal splitting of the $t_{2g}$ states of high-spin Co$^{2+}$ decreases, whereas that of low-spin Co$^{3+}$ increases and the fraction of high-spin Co$^{3+}$ increases. The results enable us to clarify the origin of the change of magnetic anisotropy and in-plane resistivity in a mixed-valence cobaltate caused by the interplay of spin-orbit coupling and tetragonal distortion.

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arXiv2021

Orbital Peierls mechanism of the formation of molecular clusters in Na2Ti3Cl8 and in similar systems

Recently the structural transition in Na2Ti3Cl8 at 200 K with the formation of triangular Ti3 clusters was studied by ab-initio calculations in PRL 124, 167203 (2020). It was concluded on the basis of the DFT+U results that the usual band effects are not sufficient to explain this transition. The authors then invoked magnetic mechanisms, including complicated factors such as biquadratic and ring exchanges. We point out that this overcomplicated description is unnecessary, and that the formation of trimers, or breathing kagome lattice in Na2Ti3Cl8, and in many other systems, has very simple, almost trivial explanation basing on the orbital-driven Peierls transition.

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arXiv2021

Multiferroics and beyond: electric properties of different magnetic textures

This article presents a survey of many nontrivial effects connected with the coupling of electric and magnetic degrees of freedom in solids -- the field initiated by I.~E.~Dzyaloshinskii in 1959. I briefly consider the main physics of ultiferroic materials, and concentrate on different effects "beyond multiferroics", based on the same physical mechanisms which operate in multiferroics. In particular they lead to nontrivial electric properties of different magnetic textures -- such as the appearance of dipoles on magnetic monopoles in spin ice, dipoles on some domain walls in the usual ferromagnets, on skyrmions etc. The inverse effect, the appearance of magnetic monopoles on electric charges in magnetoelectrics, is also discussed. This nontrivial electric activity of different magnetic textures has manifestations in many experimental properties of these materials, and it can potentially lead to novel applications.

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arXiv2021

Electric activity at magnetic moment fragmentation in spin ice

Spin ice systems display a variety of very nontrivial properties, the most striking being the existence in them of magnetic monopoles. Such monopole states can also have nontrivial electric properties: there exist electric dipoles attached to each monopole. A novel situation is encountered in the moment fragmentation (MF) state, in which monopoles and antimonopoles are perfectly ordered, whereas spins themselves remain disordered. We show that such partial ordering strongly modifies the electric activity of such systems: the electric dipoles, which are usually random and dynamic, become paired in the MF state in (d,-d) pairs, thus strongly reducing their electric activity. The electric currents existing in systems with noncoplanar spins are also strongly influenced by MF. We also consider modifications in dipole and current patterns in magnetic textures (domain walls, local defects) and at excitations with nontrivial dynamics in a MF state, which show very rich behaviour and which could in principle allow to control them by electric field.

cond-mat.str-el↗

arXiv2021

Single crystal growth and physical properties of pyroxene CoGeO$_3$

We report on the synthesis and physical properties of cm-sized CoGeO$_3$ single crystals grown in a high pressure mirror furnace at pressures of 80~bar. Direction dependent magnetic susceptibility measurements on our single crystals reveal highly anisotropic magnetic properties that we attribute to the impact of strong single ion anisotropy appearing in this system with T$_N$~$\sim$~33.5~K. Furthermore, we observe effective magnetic moments that are exceeding the spin only values of the Co ions which reveals the presence of sizable orbital moments in CoGeO$_3$.

cond-mat.mtrl-sci↗

arXiv2021

Orbital effects in solids: basics, recent progress and opportunities

The properties of transition metal compounds are largely determined by nontrivial interplay of different degrees of freedom: charge, spin, lattice, but also orbital ones. Especially rich and interesting effects occur in systems with orbital degeneracy. They result in the famous Jahn-Teller effect leading to a plethora of consequences, in static and in dynamic properties, including nontrivial quantum effects. In the present review we discuss the main phenomena in the physics of such systems, paying central attention to the novel manifestations of those. After shortly summarising the basic phenomena and their description, we concentrate on several specific directions in this field. One of them is the reduction of effective dimensionality in many systems with orbital degrees of freedom due to directional character of orbitals, with concomitant appearance of some instabilities leading in particular to the formation of dimers, trimers and similar clusters in a material. The properties of such cluster systems, largely determined by their orbital structure, are discussed in detail, and many specific examples of those in different materials are presented. Another big field which acquired special significance relatively recently is the role of relativistic spin-orbit interaction. The mutual influence of this interaction and the more traditional Jahn-Teller physics is treated in details in the second part of the review. In discussing all these questions special attention is paid to novel quantum effects in those.

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arXiv2021

Doping effects on the valence bond solid of Li$_{2}$RuO$_{3}$ with Mn substitution

$Li_{2}RuO_{3}$ with a honeycomb structure undergoes a drastic transition from a regular honeycomb lattice with the $C2/m$ space group to a valence bond solid state of the $P2_{1}/m$ space group with an extremely strong dimerization at 550 K. We synthesized $Li_{2}Ru_{1-x}Mn_{x}O_{3}$ with a full solid solution and investigated doping effects on the valence bond solid state as a function of Mn content. The valence bond solid state is found to be stable up to $x = 0.2$, based on our extensive experiments: structural studies, resistivity, and magnetic susceptibility. On the other hand, the extended x-ray absorption fine structure analyses show that the dimer local structure remains robust even above $x = 0.2$ with a minimal effect on the dimer bond length. This indicates that the locally-disordered dimer structure survives well into the Mn-rich phase even though the thermodynamically stable average structure has the $C2/m$ space group. Our results prove that the dimer formation in $Li_{2}RuO_{3}$ is predominantly a local phenomenon driven by the formation of orbitally-assisted metal-metal bonds and that these dimers are relatively robust against doping-induced disorder.

cond-mat.str-el↗

arXiv2020

Investigation of the magnetic ground state of the ordered double perovskite Sr2YbRuO6: a tale of two transitions

Comprehensive muon spin rotation/relaxation (muSR) and neutron powder diffraction (NPD) studies supported via bulk measurements have been performed on the ordered double perovskite Sr2YbRuO6 to investigate the nature of the magnetic ground state. Two sharp transitions at TN1 ~ 42 K and TN2 ~ 36 K have been observed in the static and dynamic magnetization measurements, coinciding with the heat capacity data. In order to confirm the origin of the observed phase transitions and the magnetic ground state, microscopic evidences are presented here. An initial indication of long-range magnetic ordering comes from a sharp drop in the muon initial asymmetry and a peak in the relaxation rate near TN1. NPD confirms that the magnetic ground state of Sr2YbRuO6 consists of an antiferromagnetic (AFM) structure with interpenetrating lattices of parallel Yb3+ and Ru5+ moments lying in the ab-plane and adopting a A-type AFM structure. Intriguingly, a small but remarkable change is observed in the long-range ordering parameters at TN2 confirming the presence of a weak spin reorientation (i.e. change in spin configuration) transition of Ru and Yb moments, as well as a change in the magnetic moment evolution of the Yb3+ spins at TN2. The temperature dependent behaviour of the Yb3+ and Ru5+ moments suggests that the 4d-electrons of Ru5+ play a dominating role in stabilizing the long range ordered magnetic ground state in the double perovskite Sr2YbRuO6 whereas only the Yb3+ moments show an arrest at TN2. The observed magnetic structure and the presence of a ferromagnetic interaction between Ru- and Yb- ions are explained with use of the Goodenough-Kanamori-Anderson (GKA) rules. Possible reasons for the presence of the second magnetic phase transition and of a compensation point in the magnetization data are linked to competing mechanisms of magnetic anisotropy.

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