arXiv subjects

L. Bohaty

Publications and source records attributed to L. Bohaty.

18 recordsLinked to original sources

arXiv2026

Structural studies on $A_2$ReCl$_6$ ($A$=K, Rb, Cs): absence of Jahn-Teller distortion

K$_2$ReCl$_6$ belongs to the antifluorite family and exhibits a sequence of structural transitions above the onset of magnetic order at $T_N$ = 12 K. Because of its 5d3 electronic configuration in an octahedral coordination, the ground state is a pure spin state without orbital degeneracy within the LS coupling scheme, but it can become Jahn-Teller active in the strong spin-orbit coupling limit described by the $jj$ coupling [S. Streltsov and D. I. Khomskii, Phys. Rev. X 10, 031043 (2020)]. While the structural transitions in K$_2$ReCl$_6$ are understood in terms of octahedral rotation and tilting, the possible impact of a Jahn-Teller distortion remains an open issue. We report on comprehensive crystalstructure studies by means of powder neutron and single-crystal x-ray diffraction on K$_2$ReCl$_6$ and on K$_2$SnCl$_6$. The latter material is used as a reference, because it exhibits the same sequence of structural transitions as K$_2$ReCl$_6$, but possesses a filled 4d shell ruling out a Jahn-Teller distortion. While the ReCl$_6$ octahedron in K$_2$ReCl$_6$ presents sizable distortions at intermediate temperatures, there is no such distortion persisting to low temperatures excluding a sizable Jahn-Teller effect. Studies on polycrystalline samples of Rb$_2$ReCl$_6$ and Cs$_2$ReCl$_6$, in which the structural transitions are suppressed due to the larger alkaline ionic radius, also do not find any indications for a Jahn-Teller distortion.

cond-mat.str-el↗

arXiv2023

Electronic excitations in $5d^4$ J=0 Os$^{4+}$ halides studied by RIXS and optical spectroscopy

We demonstrate that the cubic antifluorite-type halides K$_2$OsCl$_6$, K$_2$OsBr$_6$, and Rb$_2$OsBr$_6$ are excellent realizations of non-magnetic J=0 compounds. The magnetic susceptibility shows the corresponding Van-Vleck type behavior and no sign of defects. We investigate the electronic excitations with two complementary techniques, resonant inelastic x-ray scattering (RIXS) and optical spectroscopy. This powerful combination allows us to thoroughly study, e.g., on-site intra-$t_{2g}$ excitations and $t_{2g}$-to-$e_g$ excitations as well as inter-site excitations across the Mott gap and an exciton below the gap. In this way, we determine the electronic parameters with high accuracy, altogether yielding a comprehensive picture. In K$_2$OsCl$_6$, we find the spin-orbit coupling constant $ζ$=0.34 eV, Hund's coupling $J_H$=0.43 eV, the onset of excitations across the Mott gap at $Δ$=2.2 eV, the cubic crystal-field splitting 10Dq=3.3 eV, and the charge-transfer energy $Δ_{CT}$=4.6 eV. With $J_H/ζ$=1.3, K$_2$OsCl$_6$ is in the intermediate-coupling regime. In a $t_{2g}$-only Kanamori picture, the above values correspond to $ζ^{eff}$=0.41 eV and $J_H^{eff}$=0.28 eV, which is very close to results reported for related $5d^4$ iridates. In the tetragonal phase at 5 K, the non-cubic crystal field causes a peak splitting of the J=1 state as small as 4 meV. Compared to K$_2$OsCl$_6$, the bromides K$_2$OsBr$_6$ and Rb$_2$OsBr$_6$ show about 12-14 % smaller values of 10Dq and $Δ_{CT}$, while the spin-orbit-entangled intra-$t_{2g}$ excitations below 2 eV and hence $ζ$ and $J_H$ are reduced by less than 4 %. Furthermore, the Mott gap in K$_2$OsBr$_6$ is reduced to about 1.8 eV.

cond-mat.str-el↗

arXiv2023

Local symmetry breaking and low-energy continuum in K$_2$ReCl$_6 $

Using polarization selective spontaneous Raman scattering, we have investigated the 5$d$ transition metal compound K$_2$ReCl$_6$ which displays a series of structural phase transitions. We observe a violation of the Raman selection rules in the cubic high temperature phase as well as a low-energy scattering continuum persistent throughout the investigated temperature range from 300 down to 5 K. The continuum couples to one of the phonon modes at temperatures above the lowest structural phase transition at 76 K. We propose a common origin of these observations caused by local fluctuations in the orientation of the ReCl$_6$ octahedra which locally break the long-range cubic symmetry. Consistent results from the related non-magnetic compound K$_2$SnCl$_6$ support this interpretation.

cond-mat.str-el↗

arXiv2016

Strong magnetoelastic coupling at the transition from harmonic to anharmonic order in NaFe(WO$_4$)$_2$ with 3d$^5$ configuration

The crystal structure of the double tungstate NaFe(WO$_4$)$_2$ arises from that of the spin-driven multiferroic MnWO$_4$ by inserting non-magnetic Na layers. NaFe(WO$_4$)$_2$ exhibits a three-dimensional incommensurate spin-spiral structure at low temperature and zero magnetic field, which, however, competes with commensurate order induced by magnetic field. The incommensurate zero-field phase corresponds to the condensation of a single irreducible representation but it does not imply ferroelectric polarization because spirals with opposite chirality coexist. Sizable anharmonic modulations emerge in this incommensurate structure, which are accompanied by large magneto-elastic anomalies, while the onset of the harmonic order is invisible in the thermal expansion coefficient. In magnetic fields applied along the monoclinic axis, we observe a first-order transition to a commensurate structure that again is accompanied by large magneto-elastic effects. The large magnetoelastic coupling, a reduction of the $b$ lattice parameter, is thus associated only with the commensurate order. Upon releasing the field at low temperature, the magnetic order transforms to another commensurate structure that considerably differs from the incommensurate low-temperature phase emerging upon zero-field cooling. The latter phase, which exhibits a reduced ordered moment, seems to be metastable.

cond-mat.str-el↗

arXiv2014

Low-temperature ordered phases of the spin-$\frac{1}{2}$ XXZ chain system Cs$_2$CoCl$_4$

In this study the magnetic order of the spin-1/2 XXZ chain system Cs$_2$CoCl$_4$ in a temperature range from 50 mK to 0.5 K and in applied magnetic fields up to 3.5 T is investigated by high-resolution measurements of the thermal expansion and the specific heat. Applying magnetic fields along a or c suppresses $T_\textrm{N}$ completely at about 2.1 T. In addition, we find an adjacent intermediate phase before the magnetization saturates close to 2.5 T. For magnetic fields applied along b, a surprisingly rich phase diagram arises. Two additional transitions are observed at critical fields $μ_0 H_{SF1}\simeq 0.25$ T and $μ_0 H_{SF2}\simeq 0.7$ T, which we propose to arise from a two-stage spin-flop transition.

cond-mat.str-el↗

arXiv2014

Magnetoelectric properties of $A_2$[FeCl$_5$(H$_2$O)] with $A = $ K, Rb, Cs

The compounds $A_2$[FeCl$_5$(H$_2$O)] with $A=$ K, Rb, Cs are identified as new linear magnetoelectric materials. We present a detailed investigation of their linear magnetoelectric properties by measurements of pyroelectric currents, dielectric constants and magnetization. The anisotropy of the linear magnetoelectric effect of the K-based and Rb-based compound is consistent with the magnetic point group $m'm'm'$, already reported in literature. A symmetry analysis of the magnetoelectric effect of the Cs-based compound allows to determine the magnetic point group $mmm'$ and to develop a model for its magnetic structure. In addition, magnetic-field versus temperature phase diagrams are derived and compared to the closely related multiferroic (NH$_4$)$_2$[FeCl$_5$(H$_2$O)].

cond-mat.str-el↗

arXiv2014

Infrared-active phonon modes in monoclinic multiferroic MnWO4

We report on polarized infrared reflectivity measurements of multiferroic, monoclinic MnWO4 between 10K and 295K. The full dielectric tensor and the frequency dependence of the orientation of the principal axes have been determined in the frequency range of the phonons. All infrared-active phonon modes (7 A_u modes and 8 B_u modes) are unambiguously identified. In particular the strongest B_u modes have been overlooked in previous studies, in which the monoclinic symmetry was neglected in the analysis. Using a generalized Drude-Lorentz model, we determine the temperature dependence of the phonon parameters, including the orientation of the B_u modes within the ac plane. The phonon parameters and their temperature dependence have been discussed controversially in previous studies, which do not include a full polarization analysis. Our data does not confirm any of the anomalies reported above 20K. However, in the paramagnetic phase we find a drastic reduction of the spectral weights of the weakest A_u mode and of the weakest B_u mode with increasing temperature. Below 20K, the parameters of the A_u phonon modes for E||b show only subtle changes, which demonstrate a finite but weak coupling between lattice dynamics and magnetism in MnWO4. A quantitative comparison of our infrared data with the quasi-static dielectric constant epsilon_b indicates that the spectral weight of the electromagnon is tiny for E||b, in particular much smaller than the weak changes of the spectral weight of the phonons.

cond-mat.str-el↗

arXiv2014

Anisotropy study of multiferroicity in the pyroxene NaFeGe$_2$O$_6$

We present a study of the anisotropy of the dielectric, magnetic and magnetoelastic properties of the multiferroic clinopyroxene NaFeGe$_2$O$_6$. Pyroelectric currents, dielectric constants and magnetic susceptibilities as well as the thermal expansion and the magnetostriction were examined on large synthetic single crystals of NaFeGe$_2$O$_6$. The spontaneous electric polarization detected below $T_{\rm C}\simeq 11.6$ K in an antiferromagnetically ordered state ($T_{\rm N}\simeq 13$ K) is mainly lying within the $ac$ plane with a small component along $b$, indicating a triclinic symmetry of the multiferroic phase of NaFeGe$_2$O$_6$. The electric polarization can be strongly modified by applying magnetic fields along different directions. We derive detailed magnetic-field versus temperature phase diagrams and identify three multiferroic low-temperature phases, which are separated by a non-ferroelectric, antiferromagnetically ordered state from the paramagnetic high-temperature phase.

cond-mat.str-el↗

arXiv2014

Domain dynamics in the multiferroic phase of MnWO4

By using broadband linear and nonlinear dielectric spectroscopy we studied the magnetoelectric dynamics in the chiral antiferromagnet MnWO4. In the multiferroic phase the dielectric response is dominated by the dynamics of domains and domain walls which is strongly dependent on the stimulating electric field. The mean switching time reaches values in the minute range in the middle of the multiferroic temperature regime at T=10 K but unexpectedly decays again on approaching the lower, first-order phase boundary at T_N1=7.6K. The switchability of the ferroelectric domains denotes a pinning-induced threshold and can be described considering a growth-limited scenario with an effective growth dimension of d=1.8. The rise of the effective dynamical coercive field on cooling below the TN2 is much stronger compared to the usual ferroelectrics and can be described by a power law E_c ~ν^1/2. The latter questions the feasibility of fast-switching devices based on this type of material.

cond-mat.str-el↗

arXiv2014

Kinetics of the Multiferroic Switching in MnWO$_4$

The time dependence of switching multiferroic domains in MnWO$_4$ has been studied by time-resolved polarized neutron diffraction. Inverting an external electric field inverts the chiral magnetic component within rise times ranging between a few and some tens of milliseconds in perfect agreement with macroscopic techniques. There is no evidence for any faster process in the inversion of the chiral magnetic structure. The time dependence is well described by a temperature-dependent rise time suggesting a well-defined process of domain reversion. As expected, the rise times decrease when heating towards the upper boundary of the ferroelectric phase. However, switching also becomes faster upon cooling towards the lower boundary, which is associated with a first-order phase transition.

cond-mat.str-el↗

arXiv2011

Time-resolved imaging of magnetoelectric domain switching in multiferroic MnWO4

By an electrical-pump--optical-probe technique we show that the electric-field-induced reversal of the magnetic order parameter in multiferroic MnWO$_4$ occurs on the time scale of milliseconds and maintains a rigid coupling of the magnetization to the magnetically induced electric polarization. The temporal progression of the spatially resolved domain structure was imaged with nanosecond resolution by optical second harmonic generation and compared to the quasi-static domain reversal. A qualitative model gives an estimate of why the magnetoelectric order-parameter reversal in the magnetically induced ferroelectrics is not inherently ultrafast.

cond-mat.str-el↗

arXiv2010

Local symmetry and magnetic anisotropy in multiferroic MnWO4 and antiferromagnetic CoWO4 studied by soft x-ray absorption spectroscopy

Soft x-ray absorption experiments on the transition metal L2,3 edge of multiferroic MnWO4 and antiferromagnetic CoWO4 are presented. The observed linear polarization dependence, analyzed by full-multiplet calculations, is used to determine the ground state wave function of the magnetic Mn2+ and Co2+ ions. The impact of the local structure and the spin-orbit coupling on the orbital moment is discussed in terms of the single-ion anisotropy. It is shown that the orbital moment in CoWO4 is responsible for the collinear antiferromagnetism, while the small size of spin-orbit coupling effects make spiral magnetic order in MnWO4 possible, enabling the material to be multiferroic.

cond-mat.str-el↗

arXiv2010

Translation domains in multiferroics

Translation domains differing in the phase but not in the orientation of the corresponding order parameter are resolved in two types of multiferroics. Hexagonal (h-) YMnO$_3$ is a split-order-parameter multiferroic in which commensurate ferroelectric translation domains are resolved by piezoresponse force microscopy whereas MnWO$_4$ is a joint-order-parameter multiferroic in which incommensurate magnetic translation domains are observed by optical second harmonic generation. The pronounced manifestation of the generally rather "hidden" translation domains in these multiferroics and the associated drastic reduction of symmetry emphasize that the presence of translation domains must not be neglected when discussing the physical properties and functionalities of multiferroics.

cond-mat.str-el↗

arXiv2010

Second harmonic generation on incommensurate structures: The case of multiferroic MnWO4

A comprehensive analysis of optical second harmonic generation (SHG) on an incommensurate (IC) magnetically ordered state is presented using multiferroic MnWO4 as model compound. Two fundamentally different SHG contributions coupling to the primary IC magnetic order or to secondary commensurate projections of the IC state, respectively, are distinguished. Whereas the latter can be described within the formalism of the 122 commensurate magnetic point groups the former involves a breakdown of the conventional macroscopic symmetry analysis because of its sensitivity to the lower symmetry of the local environment in a crystal lattice. Our analysis thus foreshadows the fusion of the hitherto disjunct fields of nonlinear optics and IC order in condensed-matter systems.

cond-mat.str-el↗

arXiv2010

Muon-spin relaxation and heat capacity measurements on the magnetoelectric and multiferroic pyroxenes LiFeSi2O6 and NaFeSi2O6

The results of muon-spin relaxation and heat capacity measurements on two pyroxene compounds LiFeSi2O6 and NaFeSi2O6 demonstrate that despite their underlying structural similarity the magnetic ordering is considerably different. In LiFeSi2O6 a single muon precession frequency is observed below TN, consistent with a single peak at TN in the heat capacity and a commensurate magnetic structure. In applied magnetic fields the heat capacity peak splits in two. In contrast, for natural NaFeSi2O6, where multiferroicity has been observed in zero-magnetic-field, a rapid Gaussian depolarization is observed showing that the magnetic structure is more complex. Synthetic NaFeSi2O6 shows a single muon precession frequency but with a far larger damping rate than in the lithium compound. Heat capacity measurements reproduce the phase diagrams previously derived from other techniques and demonstrate that the magnetic entropy is mostly associated with the build up of correlations in the quasi-one-dimensional Fe3+ chains.

cond-mat.str-el↗

arXiv2009

Control of chiral magnetism in multiferroic MnWO4 through an electric field

The chiral components in the magnetic order in multiferroic MnWO4 have been studied by neutron diffraction using spherical polarization analysis as a function of temperature and of external electric field. We show that sufficiently close to the ferroelectric transition it is possible to switch the chiral component by applying moderate electric fields at constant temperature. Full hysteresis cycles can be observed which indicate strong pinning of the magnetic order. MnWO4, furthermore, exhibits a magnetoelectric memory effect across heating into the paramagnetic and paraelectric phase.

cond-mat.str-el↗

arXiv2007

Pyroxenes: A new class of multiferroics

Pyroxenes with the general formula $AM$Si$_2$O$_6$ ($A$ = mono- or divalent metal, $M$ = di- or trivalent metal) are shown to be a new class of multiferroic materials. In particular, we have found so far that NaFeSi$_2$O$_6$ becomes ferroelectric in a magnetically ordered state below $\simeq 6$ K. Similarly, magnetically driven ferroelectricity is also detected in the Li homologues, LiFeSi$_2$O$_6$ ($T_C \simeq 18$ K) and LiCrSi$_2$O$_6$ ($T_C \simeq 11$ K). In all these monoclinic systems the electric polarization can be strongly modified by magnetic fields. Measurements of magnetic susceptibility, pyroelectric current and dielectric constants (and their dependence on magnetic field) are performed using a natural crystal of aegirine (NaFeSi$_2$O$_6$) and synthetic crystals of LiFeSi$_2$O$_6$ and LiCrSi$_2$O$_6$ grown from melt solution. For NaFeSi$_2$O$_6$ a temperature versus magnetic field phase diagram for NaFeSi$_2$O$_6$ is proposed. Exchange constants are computed on the basis of {\it ab initio} band structure calculations. The possibility of a spiral magnetic structure caused by frustration as origin of the multiferroic behaviour is discussed. We propose that other pyroxenes may also be multiferroic, and that the versatility of this family offers an exceptional opportunity to study general conditions for and mechanisms of magnetically driven ferroelectricity.

cond-mat.str-el↗

arXiv2006

A New Multiferroic Material: MnWO4

We report the multiferroic behaviour of MnWO$_4$, a magnetic oxide with monoclinic crystal structure and spiral long-range magnetic order. Based upon recent theoretical predictions MnWO$_4$ should exhibit ferroelectric polarization coexisting with the proper magnetic structure. We have confirmed the multiferroic state below 13 K by observing a finite electrical polarization in the magnetically ordered state via pyroelectric current measurements.

cond-mat.str-el↗