arXiv subjects

M. Braden

Publications and source records attributed to M. Braden.

At least 19 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↗

arXiv2025

KOMPASS: the new cold neutron triple-axis-spectrometer specialized for polarization analysis

KOMPASS is a polarized triple-axis cold neutron spectrometer recently installed at the FRM II neutron source. The instrument is designed to operate exclusively with polarized neutrons and is specialized in longitudinal polarization analysis using Helmholtz coils and spherical zero-field neutron polarimetry using a Cryopad device. The advanced guide system polarizes and focuses flexibly in the scattering plane. A first, fixed parabolic focusing part contains a series of three polarizing supermirror V-cavities that produce a highly polarized beam. By exchanging straight and parabolic front-end guide sections, the resolution of the instrument can be optimized to meet experimental requirements. Large, double-focusing monochromator and analyzer units with pyrolytic graphite crystals enable efficient and adaptive energy selection, and a compact supermirror cavity analyzes the final neutron polarization. Alternatively, or in combination with this cavity, a Heusler polarization analyzer can be used. KOMPASS offers full- and half-polarized configurations with or without secondary energy analysis and provides a wide range of polarization options. Therefore, KOMPASS is well suited for various studies of static and dynamic magnetic correlations with energy transfers on the neutron energy loss side up to ~12 meV.

physics.ins-det↗

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-wave dispersion and magnon chirality in multiferroic TbMnO3

Inelastic neutron scattering experiments combining time-of-flight and polarized techniques yield a comprehensive picture of the magnon dispersion in multiferroic TbMnO3 including the dynamic chirality. Taking into account only Mn3+ moments, spin-wave calculations including nearest-neighbor interactions, frustrating next-nearest neighbor exchange as well as single-ion anisotropy and antisymmetric terms describe the energy dispersion and the distribution of neutron scattering intensity in the multiferroic state very well. Polarized neutron scattering reveals strong dynamic chirality of both signs that may be controlled by external electric fields in the multiferroic phase. Also above the onset of long-range multiferroic order in zero electric field, a small inelastic chiral component can be inverted by an electric field. The microscopic spin-wave calculations fully explain also the dynamic chirality of magnetic excitations, which is imprinted by the static chirality of the multiferroic phase. The ordering of Tb3+ moments at lower temperature reduces the broadening of magnons but also renders the magnon dispersion more complex.

cond-mat.str-el↗

arXiv2023

Magnon dispersion in ferromagnetic SrRuO$_3$

The magnetic excitations in ferromagnetic SrRuO$_3$ were studied by inelastic neutron scattering combining experiments on triple-axis and time-of-flight spectrometers with and without polarization analysis. A quadratic spin-wave dispersion with an anisotropy gap describes the low-energy low-temperature response. The magnon dispersion extends to at least 35 meV and there is no direct evidence for a continuum of Stoner excitations below this energy. However, the magnon response is weakened at higher energy. In addition to the anomalous softening of the spin-wave stiffness and of the gap, which is induced by the topology of the Bloch states, the magnon excitations are broadened in energy and this effect increases upon heating.

cond-mat.str-el↗

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.

cond-mat.str-el↗

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.

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↗

arXiv2021

Neutron scattering studies on spin fluctuations in Sr$_2$RuO$_4$

The magnetic excitations in Sr$_2$RuO$_4$ are studied by polarized and unpolarized neutron scattering experiments as a function of temperature. At the scattering vector of the Fermi-surface nesting with a half-integer out-of-plane component, there is no evidence for the appearance of a resonance excitation in the superconducting phase. The body of existing data indicates weakening of the scattered intensity in the nesting spectrum to occur at very low energies. The nesting signal persists up to 290 K but is strongly reduced. In contrast, a quasi-ferromagnetic contribution maintains its strength and still exhibits a finite width in momentum space.

cond-mat.supr-con↗

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↗

arXiv2020

Evidence for current-induced phase coexistence in Ca$_{2}$RuO$_{4}$ and its influence on magnetic order

Combining quasistatic and time-resolved transport measurements with X-ray and neutron diffraction experiments we study the non-equilibrium states that arise in pure and in Ti substituted Ca$_2$RuO$_4$ under the application of current densities. Time-resolved studies of the current-induced switching find a slow conductance relaxation that can be identified with heating and a fast one that unambiguously proves an intrinsic mechanism. The current-induced phase transition leads to complex diffraction patterns. Separated Bragg reflections that can be associated with the metallic and insulating phases by their lattice parameters, indicate a real structure with phase coexistence that strongly varies with temperature and current strength. A third contribution with a $c$ lattice constant in between those of metallic and insulating phases appears upon cooling. At low current densities, this additional phase appears below $\sim$100 K and is accompanied by a suppression of the antiferromagnetic order that otherwise can coexist with current carrying states. A possible origin of the intermediate phase is discussed.

cond-mat.str-el↗

arXiv2019

Strong Spin Resonance Mode associated with suppression of soft magnetic ordering in Hole-doped Ba1-xNaxFe2As2

Spin-resonance modes (SRM) are taken as evidence for magnetically driven pairing in Fe-based superconductors, but their character remains poorly understood. The broadness, the splitting and the spin-space anisotropies of SRMs contrast with the mostly accepted interpretation as spin excitons. We study hole-doped Ba$_{1-x}$Na$_x$Fe$_2$As$_2$ that displays a spin reorientation transition. This reorientation has little impact on the overall appearance of the resonance excitations with a high-energy isotropic and a low-energy anisotropic mode. However, the strength of the anisotropic low-energy mode sharply peaks at the highest doping that still exhibits magnetic ordering resulting in the strongest SRM observed in any Fe-based superconductor so far. This remarkably strong SRM is accompanied by a loss of about half of the magnetic Bragg intensity upon entering the SC phase. Anisotropic SRMs thus can allow the system to compensate for the loss of exchange energy arising from the reduced antiferromagnetic correlations within the SC state.

cond-mat.supr-con↗

arXiv2019

Spin-orbit entangled j=1/2 moments in Ba$_2$CeIrO$_6$ -- a frustrated fcc quantum magnet

We establish the double perovskite Ba$_2$CeIrO$_6$ as a nearly ideal model system for j=1/2 moments, with resonant inelastic x-ray scattering indicating a deviation of less than 1% from the ideally cubic j=1/2 state. The local j=1/2 moments form an fcc lattice and are found to order antiferromagnetically at $T_N$=14K, more than an order of magnitude below the Curie-Weiss temperature. Model calculations show that the geometric frustration of the fcc Heisenberg antiferromagnet is further enhanced by a next-nearest neighbor exchange, indicated by ab initio theory. Magnetic order is driven by a bond-directional Kitaev exchange and by local distortions via a strong magneto-elastic effect - both effects are typically not expected for j=1/2 compounds making Ba2CeIrO6 a riveting example for the rich physics of spin-orbit entangled Mott insulators.

cond-mat.str-el↗

arXiv2019

Magnetization-density distribution in the metallic ferromagnet SrRuO3 determined by polarized neutron diffraction

The magnetization-density distribution in the metallic ferromagnet SrRuO$_3$ was studied by means of polarized neutron diffraction. The analyzes by multipole refinements and by the maximum entropy method consistently reveal a strong polarization of all oxygen sites carrying 30\% of the total magnetization. The spin-density distribution on the Ru site exhibits a nearly cubic shape in agreement with an almost equal occupation of $t_{2g}$ orbitals and $pd$ hybridization. The experimental analysis is well reproduced by density functional calculations. There is no qualitative change in the magnetization distribution between 2 and 200 K.

cond-mat.str-el↗

arXiv2018

Temperature dependent percolation mechanism for conductivity in Y$_{0.63}$Ca$_{0.37}$TiO$_3$ revealed by a microstructure study

We have performed optical microscopy, micro-photoelectron spectroscopy, and micro-Raman scattering measurements on Y$_{0.63}$Ca$_{0.37}$TiO$_3$ single crystals in order to clarify the interplay between the microstructure and the temperature dependent electronic transport mechanisms in this material. Optical microscopy observations reveal dark and bright domain patterns on the surface with length scales of the order of several to a hundred micrometers showing a pronounced temperature dependent evolution. Spatially resolved photoelectron spectroscopy measurements show the different electronic character of these domains. Using micro-Raman spectroscopy, we observe a distinct temperature dependence of the crystal structure of these domains. On the basis of these findings the different domains are assigned to insulating and metallic volume fractions, respectively. By decreasing the temperature, the volume fraction of the conducting domains increases, hence allowing the electrons to percolate through the sample at temperatures lower than $\sim$150 K.

cond-mat.str-el↗

arXiv2018

Spin fluctuations in Sr2RuO4 from polarized neutron scattering: implications for superconductivity

Triplet pairing in Sr2RuO4 was initially suggested based on the hypothesis of strong ferromagnetic spin fluctuations. Using polarized inelastic neutron scattering, we accurately determine the full spectrum of spin fluctuations in Sr2RuO4. Besides the well-studied incommensurate magnetic fluctuations we do find a sizeable quasiferromagnetic signal, quantitatively consistent with all macroscopic and microscopic probes. We use this result to address the possibility of magnetically-driven triplet superconductivity in Sr2RuO4. We conclude that, even though the quasiferromagnetic signal is stronger and sharper than previously anticipated, spin fluctuations alone are not enough to generate a triplet state strengthening the need for additional interactions or an alternative pairing scenario.

cond-mat.supr-con↗