arXiv subjects

L. Bohatý

Publications and source records attributed to L. Bohatý.

15 recordsLinked to original sources

arXiv2024

Spin-orbital-lattice entanglement in the ideal j=1/2 compound K$_2$IrCl$_6$

Mott insulators with spin-orbit entangled j=1/2 moments host intriguing magnetic properties. The j=1/2 wave function requires cubic symmetry, while a noncubic crystal field mixes j=1/2 and 3/2 character. Spectroscopic studies of $5d^5$ iridates typically claim noncubic symmetry, e.g., based on a splitting of the excited j=3/2 quartet. A sizable splitting is particularly puzzling in antifluorite-type K$_2$IrCl$_6$, a frustrated fcc quantum magnet with global cubic symmetry. It raises the fundamental question about the stability of j=1/2 moments against magneto-elastic coupling. Combining resonant inelastic x-ray scattering with optical spectroscopy, we demonstrate that the multi-peak line shape in K$_2$IrCl$_6$ reflects a vibronic character of the j=3/2 states rather than a noncubic crystal field. The quasimolecular crystal structure with well separated IrCl$_6$ octahedra explains the existence of well-defined sidebands that are usually smeared out in solids. Our results highlight the spin-orbital-lattice entangled character of cubic K$_2$IrCl$_6$ with ideal j=1/2 moments.

cond-mat.str-el↗

arXiv2024

Rotational phase transitions in antifluorite-type osmate and iridate compounds

We present temperature-dependent single-crystal diffraction results on seven antifluorite-type $A_2MeX_6$ compounds with $Me$=Os or Ir: K$_2$OsCl$_6$, $A_2$OsBr$_6$ with $A$=K, Rb, Cs and NH$_4$, and K$_2$Ir$X_6$ with $X$=Cl and Br. The structural transitions in this family arise from $MeX_6$ octahedron rotations that generate a rich variety of symmetries depending on the rotation axis and stacking schemes. In order to search for local distortions in the high-symmetry phase we perform refinements of anharmonic atomic displacement parameters with comprehensive data sets. Even at temperatures close to the onset of structural distortions, these refinements only yield a small improvement indicating only small anharmonic effects. The phase transitions in these antifluorites are essentially of displacive character. However, some harmonic displacement parameters are very large reflecting soft phonon modes with the softening covering large parts of the Brillouin zone. The occurrence of the rotational transitions in the antifluorite-type family can be remarkably well analyzed in terms of a tolerance factor of ionic radii.

cond-mat.mtrl-sci↗

arXiv2023

Spin-orbit coupling in a half-filled $t_{2g}$ shell: the case of $5d^3$ K$_2$ReCl$_6$

The half-filled $t_{2g}$ shell of the $t_{2g}^3$ configuration usually, in LS coupling, hosts a S = 3/2 ground state with quenched orbital moment. This state is not Jahn-Teller active. Sufficiently large spin-orbit coupling $ζ$ has been predicted to change this picture by mixing in orbital moment, giving rise to a sizable Jahn-Teller distortion. In $5d^3$ K$_2$ReCl$_6$ we study the electronic excitations using resonant inelastic x-ray scattering (RIXS) and optical spectroscopy. We observe on-site intra-$t_{2g}$ excitations below 2 eV and corresponding overtones with two intra-$t_{2g}$ excitations on adjacent sites, the Mott gap at 2.7 eV, $t_{2g}$-to-$e_g$ excitations above 3 eV, and charge-transfer excitations at still higher energy. The intra-$t_{2g}$ excitation energies are a sensitive measure of $ζ$ and Hund's coupling $J_H$. The sizable value of $ζ\approx$ 0.29 eV places K$_2$ReCl$_6$ into the intermediate coupling regime, but $ζ/J_H \approx 0.6$ is not sufficiently large to drive a pronounced Jahn-Teller effect. We discuss the ground state wavefunction in a Kanamori picture and find that the S = 3/2 multiplet still carries about 97 % of the weight. However, the finite admixture of orbital moment allows for subtle effects. We discuss small temperature-induced changes of the optical data and find evidence for a lowering of the ground state by about 3 meV below the structural phase transitions.

cond-mat.str-el↗

arXiv2021

Multiple field-induced phases in the frustrated triangular magnet Cs$_3$Fe$_2$Br$_9$

The recently discovered material Cs$_3$Fe$_2$Br$_9$ contains Fe$_2$Br$_9$ bi-octahedra forming triangular layers with hexagonal stacking along the $c$ axis. In contrast to isostructural Cr-based compounds, the zero-field ground state is not a nonmagnetic $S=0$ singlet-dimer state. Instead, the Fe$_2$Br$_9$ bi-octahedra host semiclassical $S=5/2$ Fe$^{3+}$ spins with a pronounced easy-axis anisotropy along $c$ and interestingly, the intra-dimer spins are ordered ferromagnetically. The high degree of magnetic frustration due to (various) competing intra- and inter-dimer couplings leads to a surprisingly rich magnetic phase diagram. Already the zero-field ground state is reached via an intermediate phase, and the high-field magnetization and thermal expansion data for $H\parallel c$ identify ten different ordered phases. Among them are phases with constant magnetization of 1/3, respectively 1/2 of the saturation value, and several transitions are strongly hysteretic with pronounced length changes reflecting strong magnetoelastic coupling.

cond-mat.str-el↗

arXiv2021

Chiral Order and Multiferroic Domain Relaxation in NaFeGe$_2$O$_6$

The magnetic structure and the multiferroic relaxation dynamics of NaFeGe$_2$O$_6$ were studied by neutron scattering on single crystals partially utilizing polarization analysis. In addition to the previously reported transitions, the incommensurate spiral ordering of Fe$^{3+}$ moments in the $ac$ plane develops an additional component along the crystallographic $b$ direction below $T\approx 5\text{ K}$, which coincides with a lock-in of the incommensurate modulation. The quasistatic control of the spin-spiral handedness, respectively of the vector chirality, by external electric fields proves the invertibility of multiferroic domains down to the lowest temperature. Time-resolved measurements of the multiferroic domain inversion in NaFeGe$_2$O$_6$ reveal a simple temperature and electric-field dependence of the multiferroic relaxation that is well described by a combined Arrhenius-Merz relation, as it has been observed for TbMnO$_3$. The maximum speed of domain wall motion is comparable to the spin wave velocity.

cond-mat.str-el↗

arXiv2021

Single-crystal investigations on the multiferroic material LiFe(WO$_4$)$_2$

The crystal and magnetic structure of multiferroic LiFe(WO$_4$)$_2$ were investigated by temperature and magnetic-field dependent specific heat, susceptibility and neutron diffraction experiments on single crystals. Considering only the two nearest-neighbour magnetic interactions, the system forms a $J_1$, $J_2$ magnetic chain but more extended interactions are sizeable. Two different magnetic phases exhibiting long-range incommensurate order evolve at $T_{\text{N}1}\approx 22.2 \text{ K}$ and $T_{\text{N}2}\approx 19 \text{ K}$. First, a spin-density wave develops with moments lying in the $ac$ plane. In its multiferroic phase below $T_{\text{N}2}$, LiFe(WO$_4$)$_2$ exhibits a spiral arrangement with an additional spin-component along $b$. Therefore, the inverse Dzyaloshinskii-Moriya mechanism fully explains the multiferroic behavior in this material. A partially unbalanced multiferroic domain distribution was observed even in the absence of an applied electric field. For both phases only a slight temperature dependence of the incommensurability was observed and there is no commensurate phase emerging at low temperature or at finite magnetic fields up to $6\text{ T}$. LiFe(WO$_4$)$_2$ thus exhibits a simple phase diagram with the typical sequence of transitions for a type-II multiferroic material.

cond-mat.str-el↗

arXiv2020

Structural dimerization in the commensurate magnetic phases of NaFe(WO$_4$)$_2$ and MnWO$_4$

The structural distortion and magnetoelastic coupling induced through commensurate magnetism has been investigated by neutron diffraction in structurally related MnWO$_4$ and NaFe(WO$_4$)$_2$. Both systems exhibit a competition of incommensurate spiral and commensurate spin up-up-down-down ordering along the magnetic chains. In the latter commensurate phases, the alternatingly parallel and antiparallel arrangement of Fe$^{3+}$ respectively Mn$^{2+}$ moments leads to sizeable bond-angle modulation and thus to magnetic dimerization. For NaFe(WO$_4$)$_2$ this structural distortion has been determined to be strongest for the low-field up-up-down-down arrangement, and the structural refinement yields a bond-angle modulation of $\pm 1.15(16)$ degrees. In the commensurate phase of MnWO$_4$, superstructure reflections signal a comparable structural dimerization and thus strong magneto-elastic coupling different to that driving the multiferroic order. Pronounced anharmonic second- and third-order reflections in the incommensurate and multiferroic phase of MnWO$_4$ result from tiny commensurate fractions that can depin multiferroic domains.

cond-mat.str-el↗

arXiv2019

Resonant inelastic x-ray incarnation of Young's double-slit experiment

Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: the elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double 'slits' in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.

cond-mat.str-el↗

arXiv2017

Lattice and spin dynamics in a low-symmetry antiferromagnet NiWO$_4$

Lattice and magnetic dynamics of NiWO$_4$ single crystals were studied with the use of polarized Raman spectroscopy in a wide temperature range of 10-300 K including the antiferromagnetic ordering temperature $T_N$=62 K. Static magnetic measurements were used for characterizing the single crystals. All Raman-active phonons predicted by the group theory were observed and characterized. Magnetic symmetry analysis was used to determine possible magnetic space groups for NiWO$_4$ which can be also applied to any other isostructural crystal with the same magnetic propagation vector k=(1/2,0,0). Though the magnetic structure of NiWO$_4$ is relatively simple, a rich set of narrow and broad magnetic excitations with different polarization properties and temperature behavior in the very broad frequency range of 10-200 cm$^{-1}$ was observed, with some modes surviving at temperatures much higher than $T_N$ up to 220 K. Part of the magnetic excitations was identified as acoustic and optical spin-wave branches which allow us to construct exchange structure and estimate exchange and anisotropy constants with the use of linear spin-wave theory. Since the magnetic structure can be described as exchange-coupled AFM chains of $S=1$ ions, previously unobserved magnetic excitation at 24 cm$^{-1}$ is tentatively assigned to a Haldane gap mode.

cond-mat.mtrl-sci↗

arXiv2014

Critical slowing down near the multiferroic phase transition in MnWO$_4$

By using broadband dielectric spectroscopy in the radiofrequency and microwave range we studied the magnetoelectric dynamics in the multiferroic chiral antiferromagnet MnWO$_4$. Above the multiferroic phase transition at $T_{N2} \approx 12.6$ K we observe a critical slowing down of the corresponding magnetoelectric fluctuations resembling the soft-mode behavior in canonical ferroelectrics. This electric field driven excitation carries much less spectral weight than ordinary phonon modes. Also the critical slowing down of this mode scales with an exponent larger than one which is expected for magnetic second order phase transition scenarios. Therefore the investigated dynamics have to be interpreted as the softening of an electrically active magnetic excitation, an electromagnon.

cond-mat.str-el↗

arXiv2013

Thermodynamic properties of the new multiferroic material (NH$_4$)$_2$[FeCl$_5$(H$_2$O)]

(NH$_4$)$_2$[FeCl$_5$(H$_2$O)], a member of the family of antiferromagnetic $A_2$[Fe$X_5$(H$_2$O)] compounds ($X$ = halide ion, $A$ = alkali metal or ammonium ion) is classified as a new multiferroic material. We report the onset of ferroelectricity below ~6.9 K within an antiferromagnetically ordered state ($T_N \sim 7.25 K$). The corresponding electric polarization can drastically be influenced by applying magnetic fields. Based on measurements of pyroelectric currents, dielectric constants and magnetization we characterize the magnetoelectric, dielectric and magnetic properties of (NH$_4$)$_2$[FeCl$_5$(H$_2$O)]. Combining these data with measurements of thermal expansion, magnetostriction and specific heat, we derive detailed magnetic field versus temperature phase diagrams. Depending on the direction of the magnetic field up to three different multiferroic phases are identified, which are separated by a magnetically ordered, but non-ferroelectric phase from the paramagnetic phase. Besides these low-temperature transitions, we observe an additional phase transition at ~79 K, which we suspect to be of structural origin.

cond-mat.str-el↗

arXiv2013

The spin-$\frac{1}{2}$ XXZ chain system Cs$_2$CoCl$_4$ in a transverse magnetic field

Comparing high-resolution specific heat and thermal expansion measurements to exact finite-size diagonalization, we demonstrate that Cs$_2$CoCl$_4$ for a magnetic field along the crystallographic b axis realizes the spin-$\frac{1}{2}$ XXZ chain in a transverse field. Exploiting both thermal as well as virtual excitations of higher crystal field states, we find that the spin chain is in the XY-limit with an anisotropy $J_z/J_\perp \approx 0.12$ substantially smaller than previously believed. A spin-flop Ising quantum phase transition occurs at a critical field of $μ_0 H_b^{\rm cr} \approx 2$ T before around 3.5 T the description in terms of an effective spin-$\frac{1}{2}$ chain becomes inapplicable.

cond-mat.str-el↗

arXiv2011

The biaxial nonlinear crystal BiB3O6 as a polarization entangled photon source using non-collinear type-II parametric down-conversion

We describe the full characterization of the biaxial nonlinear crystal BiB3O6 (BiBO) as a polarization entangled photon source using non-collinear type-II parametric down-conversion. We consider the relevant parameters for crystal design, such as cutting angles, polarization of the photons, effective nonlinearity, spatial and temporal walk-offs, crystal thickness and the effect of the pump laser bandwidth. Experimental results showing entanglement generation with high rates and a comparison to the well investigated beta-BaB2O4 (BBO) crystal are presented as well. Changing the down-conversion crystal of a polarization entangled photon source from BBO to BiBO enhances the generation rate as if the pump power was increased by more than three times. Such an improvement is currently required for the generation of multiphoton entangled states.

quant-ph↗

arXiv2009

Topology and manipulation of multiferroic hybrid domains in MnWO$_4$

An investigation of the spatially resolved distribution of domains in the multiferroic phase of MnWO$_4$ reveals that characteristic features of magnetic and ferroelectric domains are inseparably entangled. Consequently, the concept of "multiferroic hybrid domains" is introduced for compounds in which ferroelectricity is induced by magnetic order. The three-dimensional structure of the domains is resolved. Annealing cycles reveal a topological memory effect that goes beyond previously reported memory effects and allows one to reconstruct the entire multiferroic multidomain structure subsequent to quenching it.

cond-mat.mtrl-sci↗

arXiv2005

Phonon modes of monoclinic BiB3O6

We present a detailed study of the phonon modes of the monoclinic compound BiB3O6 based on polarized reflectivity measurements on single crystals. The spectra are analysed by means of a generalized Drude-Lorentz model, which allows us to resolve the modes of A and B symmetry.

cond-mat.mtrl-sci↗