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Theo Siegrist

Publications and source records attributed to Theo Siegrist.

At least 19 recordsLinked to original sources
arXiv2025

Magnetic structure evolution and magnetoelastic coupling across the spin reorientation transition in TmCrO3

We present a comprehensive study of the magnetic structure evolution across the spin reorientation transition in orthorhombic (Pnma) TmCrO3. Magnetic susceptibility reveals canted antiferromagnetic (CAFM) ordering at T_N = 125 K, two compensation points (T_comp1 and T_comp2), followed by magnetization reversal with a magnetic susceptibility minimum between T_comp1 and T_comp2. Heat capacity shows a sharp lambda-type transition at T_N, associated with the long-range antiferromagnetic ordering of Cr, followed by a broad feature near 9 K. Neutron powder diffraction (NPD) establishes the Pn'm'a (Gamma2) magnetic structure below T_N. A gradual change in magnetic structure occurs during the spin-reorientation (SRO) transition below 30 K, where the magnetic symmetry transforms from Pn'm'a (Gamma2) to Pn'ma' (Gamma4) phase. However, below the SRO, neither Gamma2 nor Gamma4 alone adequately fit the intensity of magnetic reflections. A satisfactory refinement is achieved using the monoclinic subgroup P21'/c', derived from a combination of Gamma2 and Gamma4. The gradual SRO of Tm and Cr moments across the compensation regime is consistent with the magnetic symmetry P21'/c'. Furthermore, the ordered moments of Cr and Tm in TmCrO3 exhibit a complex, non-monotonic temperature dependence, with the Tm sublattice driving the spin-reorientation transition near the compensation point. Anomalies in the lattice parameters reveal strong magnetoelastic coupling, linking structural distortions to the SRO.

cond-mat.str-el↗
arXiv2025

Magnetically Assisted Separation of Weakly Magnetic Metal Ions in Porous Media. Part 2: Numerical Simulations

We present a numerical investigation of the magnetophoresis of metal ions in porous media under static, nonuniform magnetic fields. The multiphysics simulations couple momentum transport, mass diffusion, and magnetic field equations, with the porous medium modeled using two distinct approaches: a Stokes-based formulation incorporating effective diffusivity, and a Brinkman-based formulation that explicitly accounts for permeability and medium-induced drag. Comparison with recent experimental data [Nwachuwku et al. Submitted, 2025] reveals that the Stokes model partially fails to capture key trends, while the Brinkman model, with permeability accurately reproduces observed transport behavior on various porous media. Our simulations predict that both paramagnetic (MnCl2) and diamagnetic (ZnCl2) ions may form field-induced clusters under magnetic gradients over a range of concentrations of 1mM-100mM and magnetic field gradients of up to 100 T2/m. The dominant driving force is found to be the magnetic gradient (Kelvin) force, while the paramagnetic force from concentration gradients contributes minimally. In binary mixtures, hydrodynamic interactions between paramagnetic and diamagnetic clusters significantly alter transport dynamics. Specifically, paramagnetic clusters can pull diamagnetic clusters along the magnetic field gradient, enhancing diamagnetic migration and suppressing the motion of paramagnetic species. These findings highlight the importance of porous media modeling and interspecies interactions in predicting magnetophoretic transport of ionic mixtures.

physics.chem-ph↗
arXiv2025

Magnetically Assisted Separation of Weakly Magnetic Metal Ions in Porous Media.Part 1: Experiments

We report experiments on the magnetophoresis of paramagnetic (MnCl2) and diamagnetic (ZnCl2) metal ions in porous media under the influence of a non-uniform magnetic field generated by a permanent magnet. Experiments were carried out in a range of initial ion concentrations (1-100 mM), porous media particle sizes (63 um and 500 um), and varying mixture ratios of metal ion concentrations. For single-ion magnetophoresis, paramagnetic MnCl2 migrated toward the magnet surface, with an enrichment of approximately 2-4 percent near regions of high magnetic field. Conversely, diamagnetic ZnCl2 moved away from regions of highest magnetic field gradients, with depletion levels of 0.5-1.8 percent relative to the initial concentration. Our results demonstrate that magnetophoresis is directly proportional to porous media particle size, increasing with larger particle sizes, a trend attributed to the reduced drag forces experienced by the ions in media with larger particles. Interestingly, in binary mixtures, both MnCl2 and ZnCl2 migrated toward regions of highest magnetic field, contrary to their individual behaviors. The magnetophoretic effect of MnCl2 was diminished with increasing concentrations of ZnCl2, indicating interactions between the two ions. These findings suggest that both metal ions undergo field-induced cluster formation, with cluster sizes in the micrometer range, in both single and binary ion systems. In binary mixtures, the two ions appear to interact, potentially forming mixed clusters containing both MnCl2 and ZnCl2.

cond-mat.mtrl-sci↗
arXiv2025

Structural Inhomogeneities and Suppressed Magneto-Structural Coupling in Mn-Substituted GeCo2O4

A comprehensive study of Ge1-xMnxCo2O4 (GMCO) system was conducted using neutron powder diffraction (NPD), x-ray diffraction (XRD), Scanning electron microscopy, magnetometry, and heat capacity measurements. Comparative analysis with GeCo2O4 (GCO) highlights the influence of Mn substitution on the crystal and magnetic structure at low temperature. Surprisingly, phase separation is observed in GMCO with a targeted nominal composition of Ge0.5Mn0.5Co2O4. SEM/EDX analysis reveals that the sample predominantly consists of a Mn-rich primary phase with approximate stoichiometry Mn0.74Ge0.18Co2O4, along with a minor Ge-rich secondary phase of composition Ge0.91Mn0.19Co2O4. Although both GCO and GMCO crystallize in cubic symmetry at room temperature, a substantial difference in low-temperature structural properties has been observed. Magnetic and heat capacity data indicate ferrimagnetic ordering in the Mn-rich phase near TC = 108 K, while the Ge-rich phase exhibits antiferromagnetic order at TN = 22 K in GMCO. Analysis of heat capacity data reveals that the estimated magnetic entropy amounts to only 63% of the theoretical value expected in GMCO. A collinear ferrimagnetic arrangement is observed in the Mn rich phase below the magnetic ordering temperature, characterized by antiparallel spins of the Mn at A site and Co at B site along the c-direction. At 5 K, the refined magnetic moments are 2.31(3) for MnA and 1.82(3) uB for CoB in the Mn rich ferrimagnetic phase. The magnetic structure at 5 K in the Ge rich secondary phase is identical to the antiferromagnetic structure of the parent compound GeCo2O4. The refined value of the CoB moment in this phase at 5 K is 2.53(3) uB.

cond-mat.mtrl-sci↗
arXiv2025

Magnetophoresis of Weakly Magnetic Nanoparticle Suspension Around a Wire

We present a combined experimental and numerical study into the magnetophoresis behavior of weakly magnetic nanoparticle suspensions in the vicinity of a wire under a non-uniform magnetic field and negligible inertia. The experiments were conducted within a closed rectangular cuvette, with a wire positioned between the poles of an electromagnet. Two types of nanoparticles, paramagnetic manganese oxide and diamagnetic bismuth oxide, were studied across a broad range of concentrations (10-100 mgL), magnetic field strengths (0.25-1 T), and wire diameters (0.8-3.17 mm). Our experimental findings reveal that upon the application of a magnetic field, paramagnetic nanoparticles experience a strong, attractive force toward the wire periphery. This force generates vortices and secondary flows around the wire, depleting particles from the bulk of the cuvette and concentrating them near the wire surface. The magnetophoresis dynamics of paramagnetic nanoparticles are shown to scale with their initial concentration, wire diameter, and the strength of the external magnetic field. In contrast, diamagnetic nanoparticles exhibit markedly different behavior, with their magnetophoresis dynamics showing minimal dependence on initial concentration and magnetic field strength, while being inversely proportional to the wire diameter. Multiphysics numerical simulations complement the experimental observations, revealing the formation of field-induced particle clusters in weakly paramagnetic nanoparticles, which enhance magnetophoresis. Additionally, the critical magnetic field threshold for the onset of cluster formation is found to be lower than those predicted by theoretical models for clustering in uniform magnetic fields. Under specific conditions, including high magnetic field strengths and elevated nanoparticle concentrations, diamagnetic nanoparticles appear to undergo field-induced clustering.

cond-mat.mtrl-sci↗
arXiv2025

Magnetophoresis of paramagnetic nanoparticles in suspensions under magnetic field gradients

We systematically investigate the magnetophoresis of weakly paramagnetic manganese oxide nanoparticles under nonuniform magnetic fields using a combination of experiments and multiphysics numerical simulations. Experiments were conducted in a closed cuvette exposed to a nonuniform magnetic field generated by an electromagnet, covering a wide range of particle concentrations 25-200 mgL and magnetic field gradients 0-110 T2m. The experimental results reveal that paramagnetic manganese oxide nanoparticles exhibit significant magnetophoretic behavior, leading to particle depletion within the cuvette. The depletion rate is independent of the initial particle concentration but strongly depends on the magnetic field gradient. At low magnetic field gradients, magnetophoresis progresses slowly, while at higher gradients, the particle depletion rate increases significantly before stabilizing. Transient concentration gradients emerge within the cuvette during magnetophoresis, which we hypothesize are driven by magnetic Grashof numbers near unity. When magnetic Grashof is beyond 1, the formation of concentration gradients induces bulk fluid flows that accelerate particle capture at regions of maximum magnetic field strength. In systems where magnetophoresis opposes sedimentation, particle depleted regions form when the ratio of magnetic to gravitational Peclet numbers exceeds 1. The numerical simulations suggest formation field induced aggregation for manganese oxide nanoparticles with radii of 130 nm or larger. These insights highlight the potential of magnetic separation for sustainable metal recovery, offering a scalable and environmental friendly solution for recycling critical materials from spent electronics.

cond-mat.mtrl-sci↗
arXiv2025

Dynamics of Transition Metal Ion Transport in High-Gradient Magnetic Fields

Magnetic separation has emerged as an eco-friendly and sustainable technique with applications in water purification, chemical separation, biochemical, medical, and mining. In this study, we present, a combined experimental and theoretical investigation of the transport of transition metal ions using high-gradient magnetic fields. Experiments were conducted on aqueous solutions containing either paramagnetic manganese chloride (MnCl$_$2) or diamagnetic zinc chloride (ZnCl$_$2) ions, with concentrations ranging from 1 mM to 100 mM under a non-uniform magnetic field of an electromagnet. Our results demonstrate that while paramagnetic MnCl$_$2 is captured by the mesh wool in the magnetic field, diamagnetic ZnCl$_$2 remains unaffected by the presence of magnetic field. The capture efficiency of paramagnetic MnCl$_$2 increases with both the initial ion concentration and the applied magnetic field strength. Furthermore, in binary mixtures, the capture rate of MnCl2 is reduced compared to single-ion solutions, highlighting the role of ion interactions in magnetic separation. Our theoretical modeling indicates that magnetic capture is governed by a balance between magnetic forces and viscous forces. Additionally, the magnetic separation process is enhanced by the field-induced cluster formation of paramagnetic metal ions, which are predicted to be two orders of magnitude larger than individual hydrated ion units. These findings provide insights into the mechanisms of magnetic transport of metal ions and offer potential pathways for improving separation efficiency in complex ion mixtures that contain critical materials.

cond-mat.mtrl-sci↗
arXiv2024

Magneto-optical evidence of tilting effect in coupled Weyl bands

Theories have revealed the universality of the band tilting effect in topological Weyl semimetals (WSMs) and its implications for the material's physical properties. However, the experimental identification of tilted Weyl bands remains much less explored. Here, by combining magneto-infrared optical studies with a four-band coupled Weyl point model, we report spectroscopic evidence of the tilting effect in the well-established WSM niobium phosphide. Specifically, we observe Landau level transitions with rich features that are well reproduced within a model of coupled tilted Weyl points. Our analysis indicates that the tilting effect relaxes the selection rules and gives rise to transitions that would otherwise be forbidden in the non-tilt case. Additionally, we observe unconventional interband transitions with flat and negative magnetic field dispersions, highlighting the importance of coupling between Weyl points. Our results not only emphasize the significance of the tilting effect in the optical responses of WSMs but also demonstrate magneto-optics as an effective tool for probing the tilting effect in electronic band structures.

cond-mat.mtrl-sci↗
arXiv2022

Investigation of the monopole magneto-chemical potential in spin ices using capacitive torque magnetometry

The single-ion anisotropy and magnetic interactions in spin-ice systems give rise to unusual non-collinear spin textures, such as Pauling states and magnetic monopoles. The effective spin correlation strength ($J_{eff}$) determines the relative energies of the different spin-ice states. With this work, we display the capability of capacitive torque magnetometry in characterizing the magneto-chemical potential associated with monopole formation. We build a magnetic phase diagram of Ho$_2$Ti$_2$O$_7$, and show that the magneto-chemical potential depends on the spin-sublattice ($α$ or $β$), i.e., the Pauling state, involved in the transition. Monte-Carlo simulations using the dipolar-spin-ice Hamiltonian support our findings of a sublattice-dependent magneto-chemical potential, but the model underestimates the $J_{eff}$ for the $β$-sublattice. Additional simulations, including next-nearest neighbor interactions ($J_2$), show that long-range exchange terms in the Hamiltonian are needed to describe the measurements. This demonstrates that torque magnetometry provides a sensitive test for $J_{eff}$ and the spin-spin interactions that contribute to it.

cond-mat.str-el↗
arXiv2020

Orbital Fingerprint of Topological Fermi Arcs in a Weyl Semimetal

The monopnictides TaAs and TaP are well-established Weyl semimetals. Yet, a precise assignment of Fermi arcs, accomodating the predicted chiral charge of the bulk Weyl points, has been difficult in these systems, and the topological character of different surface features in the Fermi surface is not fully understood. Here, employing a joint analysis from linear dichroism in angle-resolved photoemission and first-principles calculations, we unveil the orbital texture on the full Fermi surface of TaP(001). We observe pronounced switches in the orbital texture at the projectedWeyl nodes, and show how they facilitate a topological classification of the surface band structure. Our findings establish a critical role of the orbital degrees of freedom in mediating the surface-bulk connectivity in Weyl semimetals.

cond-mat.str-el↗
arXiv2019

Modification of Spin Ice Physics in Ho$_2$Ti$_2$O$_7$ Thin Films

We present an extensive study on the effect of substrate orientation, strain, stoichiometry and defects on spin ice physics in Ho$_2$Ti$_2$O$_7$ thin films grown onto yttria-stabilized-zirconia substrates. We find that growth in different orientations produces different strain states in the films. All films exhibit similar c-axis lattice parameters for their relaxed portions, which are consistently larger than the bulk value of 10.10 Å. Transmission electron microscopy reveals anti-site disorder and growth defects to be present in the films, but stuffing is not observed. The amount of disorder depends on the growth orientation, with the (110) film showing the least. Magnetization measurements at 1.8 K show the expected magnetic anisotropy and saturation magnetization values associated with a spin ice for all orientations; shape anisotropy is apparent when comparing in and out-of-plane directions. Significantly, only the (110) oriented films display the hallmark spin ice plateau state in magnetization, albeit less well-defined compared to the plateau observed in a single crystal. Neutron scattering maps on the more disordered (111) oriented films show the Q=0 phase previously observed in bulk materials, but the Q=X phase giving the plateau state remains elusive. We conclude that the spin ice physics in thin films is modified by defects and strain, leading to a reduction in the temperature at which correlations drive the system into the spin ice state.

cond-mat.str-el↗
arXiv2019

Mini Volume Collapse as Evidence for a 3-Body Magnetic Polaron in $Sm_{1-x}Eu_xS$

Samarium sulfide (SmS) is a non-magnetic narrow-gap (0.06 eV) semiconductor which undergoes a transition to a metallic intermediate valence state at 6.5 kbar. Europium sulfide (EuS) is a ferromagnetic semiconductor with a Curie temperature of 16K and a gap of 1.6 eV. Here we present a study of the lattice constant, magnetic susceptibility, and resistivity of the substitution series $Sm_{1-x}Eu_xS$ for 0 < x < 1. We observe a smooth interpolation of magnetic and transport behavior across the series, consistent with a virtual crystal scenario and Vegard's law. Surprisingly, however, the lattice constant deviates below Vegard's law in a manner that suggests parametric control of the Sm-Sm distance by the Eu moment in the manner of a magnetic polaron.

cond-mat.mes-hall↗
arXiv2018

Uncovering the Origin of Divergence in the CsM(CrO$_4$)$_2$ (M = La, Pr, Nd, Sm, Eu; Am) Family through Examination of the Chemical Bonding in a Molecular Cluster and by Band Structure Analysis

A series of f-block chromates, CsM(CrO$_4$)$_2$ (M = La, Pr, Nd, Sm, Eu; Am), were prepared revealing notable differences between the AmIII derivatives and their lanthanide analogs. While all compounds form similar layered structures, the americium compound exhibits polymorphism and adopts both a structure isomorphous with the early lanthanides as well as one that possesses lower symmetry. Both polymorphs are dark red and possess band gaps that are smaller than the LnIII compounds. In order to probe the origin of these differences, the electronic structure of $α$-CsSm(CrO$_4$)$_2$, $α$-CsEu(CrO$_4$)$_2$ and $α$-CsAm(CrO$_4$)$_2$ were studied using both a molecular cluster approach featuring hybrid density functional theory and QTAIM analysis, and by the periodic LDA+GA and LDA+DMFT methods. Notably, the covalent contributions to bonding by the f orbitals was found to be more than twice as large in the AmIII chromate than in the SmIII and EuIII compounds, and even larger in magnitude than the Am-5f spin-orbit splitting in this system. Our analysis indicates also that the Am-O covalency in $α$-CsAm(CrO$_4$)$_2$ is driven by the degeneracy of the 5f and 2p orbitals, and not by orbital overlap.

cond-mat.str-el↗
arXiv2016

Growth of EuO single crystals at reduced temperatures

Single crystals of (Eu$_{1-x}$Ba$_x$)O have been grown in a molten barium-magnesium metal flux at temperatures up to 1000°C, producing single crystals of (Eu$_{1-x}$Ba$_x$)O with barium doping levels ranging from $x=0.03$ to $x=0.25$. Magnetic measurements show that the ferromagnetic Curie temperature T$_C$ correlates with the Ba doping levels, and a modified Heisenberg model was used to describe the stoichiometry dependence of T$_C$. Extrapolation of the results indicates that a sample with Ba concentration of $x=0.72$ should have a T$_C$ of 0 K, potentially producing a quantum phase transition in this material.

cond-mat.mtrl-sci↗
arXiv2016

Thermodynamic Measurement of Angular Anisotropy at the Hidden Order Transition of URu$_2$Si$_2$

The heavy fermion compound URu$_2$Si$_2$ continues to attract great interest due to the unidentified hidden order it develops below 17.5K. The unique Ising character of the spin fluctuations and low temperature quasiparticles is well established. We present detailed measurements of the angular anisotropy of the nonlinear magnetization that reveal a $\cos^4 θ$ Ising anisotropy both at and above the ordering transition. With Landau theory, we show this implies a strongly Ising character of the itinerant hidden order parameter.

cond-mat.str-el↗
arXiv2016

Competing covalent and ionic bonding in Ge-Sb-Te phase change materials

Ge2Sb2Te5 and related phase change materials are highly unusual in that they can be readily transformed between amorphous and crystalline states using very fast melt, quench, anneal cycles, although the resulting states are extremely long lived at ambient temperature. These states have remarkably different physical properties including very different optical constants in the visible in strong contrast to common glass formers such as silicates or phosphates. This behavior has been described in terms of resonant bonding, but puzzles remain, particularly regarding different physical properties of crystalline and amorphous phases. Here we show that there is a strong competition between ionic and covalent bonding in cubic phase providing a link between the chemical basis of phase change memory property and origins of giant responses of piezoelectric materials (PbTiO3, BiFeO3). This has important consequences for dynamical behavior in particular leading to a simultaneous hardening of acoustic modes and softening of high frequency optic modes in crystalline phase relative to amorphous. This different bonding in amorphous and crystalline phases provides a direct explanation for different physical properties and understanding of the combination of long time stability and rapid switching and may be useful in finding new phase change compositions with superior properties.

cond-mat.mtrl-sci↗
arXiv2015

Non-stoichiometry and Defects in the Weyl Semimetals TaAs, TaP, NbP, and NbAs

We report a structural study of the Weyl semimetals TaAs, TaP, NbP, and NbAs, utilizing diffraction techniques (single crystal x-ray diffraction and energy dispersive spectroscopy) and imaging techniques (transmission electron microscopy/scanning transmission electron microscopy). We observe defects of various degrees, leading to non-stoichiometric single crystals of all four semimetals. While TaP displays a large pnictide deficiency with composition TaP$_{0.83(3)}$, and stacking faults accompanied by anti-site disorder and site vacancies, TaAs displays transition metal deficiency with composition Ta$_{0.92(2)}$As and a high density of stacking faults. NbP also displays pnictide deficiency, yielding composition NbP$_{0.95(2)}$, and lastly, NbAs display very little deviation from a 1:1 composition, NbAs$_{1.00(3)}$, and is therefore recommended to serve as the model compound for these semimetals.

cond-mat.mtrl-sci↗