arXiv subjects

S. Süllow

Publications and source records attributed to S. Süllow.

At least 19 recordsLinked to original sources

arXiv2026

Competing Ordering Modes in the Distorted Quantum Kagome Material Clinoatacamite Cu$_2$Cl(OH)$_3$

We have studied the magnetic properties of clinoatacamite Cu$_2$Cl(OH)$_3$, the parent compound of the quantum spin liquid candidate herbertsmithite and a longstanding puzzle among frustrated quantum magnets. As we reveal using density-functional theory, clinoatacamite belongs to the class of distorted kagome antiferromagnets with the kagome plane being embedded into a low-symmetry crystal structure. By means of thermodynamic measurements, muon spin rotation/relaxation as well as neutron diffraction on single crystals, we find in zero magnetic field complex behavior below $T_\mathrm{I}$ = 18.1 K which unfolds in three temperature regions I-III. We propose this complexity in multicritical clinoatacamite to arise from the competition of antiferromagnetic ordering modes from the underconstrained manifold of modes, which can lead to a metamagnetic texture in zero field.

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arXiv2026

The Magnetic Ground State of Atacamite Cu$_2$Cl(OH)$_3$: The Crucial Role of Frustrated Zigzag Chains Revealed by Inelastic Neutron Scattering

We report inelastic neutron scattering (INS) measurements on the magnetically frustrated $S=\frac12$ sawtooth-chain compound atacamite Cu$_2$Cl(OH)$_3$ featuring inequivalent Cu(1) and Cu(2) sites. Transverse to the sawtooth chains, INS reveals two dispersive spin-wave modes and a gap of at least 0.75 meV. This behavior is rationalized within a zigzag-chain model of Cu(2) spins in an effective magnetic field of Cu(1) spins. The model is compatible with first-principles calculations and accounts for INS dispersions within linear spin-wave theory calculations. Our results reveal a unique case of an effective separation of energy scales between two differently oriented one-dimensional chains, with the zigzag-chain model being essential to fully characterize atacamite's low-energy magnetism.

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arXiv2025

Cubic magnetic anisotropy in $B$20 magnets: Interplay of anisotropy and magnetic order in Fe$_{1-x}$Co$_{x}$Si

The metallic systems MnSi and Fe$_{1-x}$Co$_{x}$Si are known to feature a generic magnetic phase diagram primarily determined by the isotropic exchange and Dzyaloshinskii-Moriya interactions. However, additional weaker anisotropies, lowest in the hierarchy of energy scales, play a crucial role: they determine the relative order of phases in the phase diagram and may even enable skyrmion stability far below the ordering temperature. Among cubic B20 helimagnets, the insulator Cu$_2$OSeO$_3$ is currently the only known example exhibiting a low-temperature, anisotropy-induced skyrmion pocket. In this manuscript, we present a systematic study of cubic magnetocrystalline anisotropy by means of angle-resolved SQUID magnetization measurements in MnSi and Fe$_{1-x}$Co$_{x}$Si ($0.08 \leq x \leq 0.70$) single crystals and provide quantitative values of the anisotropy constants. For Fe$_{1-x}$Co$_{x}$Si, the cubic anisotropy is found to be strongly dependent on the Co concentration $x$. In particular, for low Co concentrations ($x \sim 0.10$), the anisotropy is sufficiently strong to stabilize a low-temperature skyrmion lattice, in agreement with theoretical predictions. This finding suggests that Fe$_{1-x}$Co$_{x}$Si may represent the first chiral metallic system to exhibit a low-temperature skyrmion phase controllably stabilized by cubic anisotropy for specific directions of the magnetic field.

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arXiv2025

Low-Temperature Skyrmions and Spiral Reorientation Processes in Chiral Magnets with Cubic Anisotropy: Guidelines for Bridging Theory and Experiment

We revisit the phenomenological Dzyaloshinskii framework, a central theoretical approach for describing magnetization processes in bulk chiral magnets, and demonstrate how magnetocrystalline cubic anisotropy reshapes the phase diagrams of states and provides the key mechanism stabilizing low-temperature skyrmion phases. We show that, for magnetic field directions along the easy anisotropy axes, the phase diagrams feature stable skyrmion pockets for both signs of the anisotropy constant. We further analyze the nature of the transitions at the critical field $H_{c1}$, associated with the reorientation of stable and metastable spirals along the field. We also examine the transition at $H_{c2}$, where the conical state closes into the homogeneous state accompanied by a deviation of the wave vector from the field direction. By mapping characteristic anisotropy-dependent parameters in the theoretical phase diagrams, we provide guidelines for connecting theory with experiment and for estimating the cubic anisotropy constant in Fe$_{1-x}$Co$_x$Si and MnSi. Our results indicate that samples Fe$_{1-x}$Co$_x$Si with small $x \sim 0.1$ possess sufficiently strong cubic anisotropy to stabilize a low-temperature skyrmion phase. Overall, these theoretical findings establish a quantitative framework for predicting and interpreting skyrmion stability in other cubic helimagnets as well.

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arXiv2025

Atacamite Cu$_2$Cl(OH)$_3$ in High Magnetic Fields: Quantum Criticality and Dimensional Reduction of a Sawtooth-Chain Compound

We report an extensive high-field study of atacamite Cu$_2$Cl(OH)$_3$, a material realization of quantum sawtooth chains with weak interchain couplings, in continuous and pulsed magnetic fields up to 58 T. In particular, we have mapped the entropy landscape for fields as high as 35 T and have identified a field-induced quantum critical point at 21.9(1) T for $\mathbf{H} \parallel c$ axis. The quantum critical point separates field regions with and without magnetic order, evidenced by our thermodynamic study and $^1$H nuclear magnetic resonance spectroscopy, but lies far below full saturation of the magnetization. Corroborated by numerical results using density-matrix renormalization group (DMRG) calculations, we find this behavior associated with a dimensional reduction of the spin system: the sawtooth chain effectively decouples into an antiferromagnetic spin-$1/2$ chain (backbone of the sawtooth chain) in the presence of an exchange field produced by the remaining field-polarized spins.

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arXiv2023

Near coincidence of metal-insulator transition and quantum critical fluctuations: Electronic ground state and magnetic order in Fe$_{1-x}$Co$_{x}$Si

We present a detailed study of the electronic and magnetic ground state properties of Fe$_{1-x}$Co$_{x}$Si using a combination of macroscopic and microscopic experimental techniques. From these experiments we quantitatively characterize the metal-insulator transition and magnetic/non-magnetic quantum phase transition occurring at low doping levels in Fe$_{1-x}$Co$_{x}$Si. From our study, we find a surprising closeness of the critical composition of the metal-insulator transition at $x_{\mathrm{MIT}} = 0.014$ and the quantum phase transition at $x_{\mathrm{LRO}} \sim 0.024-0.031$. It suggests that these effects are cooperative and depend on each other.

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arXiv2022

From spin liquid to magnetic ordering in the anisotropic kagome Y-Kapellasite Y3Cu9(OH)19Cl8: a single crystal study

Y3Cu9(OH)19Cl8 realizes an original anisotropic kagome model hosting a rich magnetic phase diagram [M. Hering et al, npj Computational Materials 8, 1 (2022)]. We present an improved synthesis of large phase-pure single crystals via an external gradient method. These crystals were investigated in details by susceptibility, specific heat, thermal expansion, neutron scattering and local muSR and NMR techniques. At variance with polycristalline samples, the study of single crystals gives evidence for subtle structural instabilities at 33K and 13K which preserve the global symmetry of the system and thus the magnetic model. At 2.1K the compound shows a magnetic transition to a coplanar (1/3,1/3) long range order as predicted theoretically. However our analysis of the spin wave excitations yields magnetic interactions which locate the compound closer to the phase boundary to a classical jammed spin liquid phase. Enhanced quantum fluctuations at this boundary may be responsible for the strongly reduced ordered moment of the Cu2+, estimated to be 0.075muB from muSR.

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arXiv2022

Muon spin rotation and relaxation study on Nb$_{1-y}$Fe$_{2+y}$

We present a detailed study of the magnetic properties of weakly ferromagnetic/quantum critical Nb$_{1-y}$Fe$_{2+y}$ using muon spin rotation and relaxation ($μ$SR). By means of an angular dependent study of the muon spin rotation signal in applied magnetic fields on a single crystal in the paramagnetic state we establish the muon stopping site in the crystallographic lattice of NbFe$_2$. With this knowledge we develop models to describe the muon spin rotation and relaxation signals in the weakly ferromagnetic, spin density wave and quantum critical phases of Nb$_{1-y}$Fe$_{2+y}$ and fit the corresponding experimental data. In particular, we quantify the $μ$SR response for quantum critical behavior in Nb$_{1.0117}$Fe$_{1.9883}$ and extract the influence of residual weak structural disorder. From our analysis, Nb$_{1-y}$Fe$_{2+y}$ emerges to be uniquely suited to study quantum criticality close to weak itinerant ferromagnetic order.

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arXiv2022

Low-energy spin excitations of the frustrated ferromagnetic $J_1$-$J_2$ chain material linarite, PbCuSO$_4$(OH)$_2$, in applied magnetic fields $\mathbf{H} \parallel b$ axis

We report a study of the spin dynamics of the frustrated ferromagnetic $J_1$-$J_2$ chain compound linarite, PbCuSO$_4$(OH)$_2$, in applied magnetic fields up to field polarization. By means of an extreme-environment inelastic neutron scattering experiment, we have measured the low-energy spin excitations of linarite in fields up to 8.8 T for $\mathbf{H} \parallel b$ axis. We have recorded the spin excitation spectra along $h$, $k$ and $l$ for the field-induced magnetic phases IV, V and the field polarized state close to saturation. By employing first-principles calculations, we estimate the leading magnetic exchanges out of the $bc$ plane and model the dispersion relations using linear spin-wave theory. In this way, we find evidence for a (very weak) residual magnetic exchange coupling out of the $bc$ plane. Together with the previously established dominant intrachain couplings $J_1$ and $J_2$ and the interchain coupling $J_3$, we derive an effective set of exchange couplings for a microscopic description of linarite. Further, we find that the peculiar character of phase V manifests itself in the measured spin dynamics.

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arXiv2021

Crystallographic and magnetic structure of UNi$_4$$^{11}$B

We present an extensive powder and single-crystal neutron scattering investigation of the crystallographic structure and magnetic order of the frustrated metallic $f$-electron magnet UNi$_4$B. We carry out a full refinement of the crystallographic structure and conclude that the low-temperature lattice symmetry is orthorhombic (space group Pmm2; cell parameters: $a = 6.963(4)~Å$ , $b = 14.793(9)~Å$ , $c = 17.126(8)~Å$). We determine the magnetically ordered structure, concluding that below $T_\mathrm{N} = 19.5~\mathrm{K}$ the material undergoes a transition into a partially ordered antiferromagnetic state. The magnetic structure is consistent with the existence of toroidal order in this material. We further test the proposal of a second magnetic transition occurring at $330~\mathrm{mK}$, concluding that the thermodynamic anomalies observed at these temperatures do not reflect modifications of the magnetic structure. Our study provides a consistent picture of the interrelationship of structural and magnetic properties in the frustrated magnet UNi$_4$B previously unresolved.

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arXiv2021

Magnetization process of atacamite: a case of weakly coupled $S = 1/2$ sawtooth chains

We present a combined experimental and theoretical study of the mineral atacamite Cu$_2$Cl(OH)$_3$. Density functional theory yields a Hamiltonian describing anisotropic sawtooth chains with weak 3D connections. Experimentally, we fully characterize the antiferromagnetically ordered state. Magnetic order shows a complex evolution with the magnetic field, while, starting at 31.5 T, we observe a plateau-like magnetization at about $M_{\rm sat}/2$. Based on complementary theoretical approaches, we show that the latter is unrelated to the known magnetization plateau of a sawtooth chain. Instead, we provide evidence that the magnetization process in atacamite is a field-driven canting of a 3D network of weakly coupled sawtooth chains that form giant moments.

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arXiv2020

Magnetic and electronic phases of U$_\mathbf{2}$Rh$_\mathbf{3}$Si$_\mathbf{5}$

We present a detailed study of the magnetic and electronic properties of U$_2$Rh$_3$Si$_5$, a material that has been demonstrated to exhibit a first order antiferromagnetic phase transition. From a high magnetic field study, together with extensive experiments in moderate fields, we establish the magnetic phase diagrams for all crystallographic directions. The possibility of an electronic phase in a narrow interval above the Néel temperature as a precursor of a magnetic phase is discussed.

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arXiv2019

The magnetic phase diagram of the frustrated spin chain compound linarite, PbCuSO$_4$(OH)$_2$, as seen by neutron diffraction and $^1$H-NMR

We report on a detailed neutron diffraction and $^1$H-NMR study on the frustrated spin-1/2 chain material linarite, PbCuSO$_4$(OH)$_2$, where competing ferromagnetic nearest neighbor and antiferromagnetic next-nearest neighbor interactions lead to frustration. From the magnetic Bragg peak intensity studied down to 60 mK, the magnetic moment per Cu atom is obtained within the whole magnetic phase diagram for $H \parallel b$ axis. Further, we establish the detailed configurations of the shift of the SDW propagation vector in phase V with field and temperature. Finally, combining our neutron diffraction results with those from a low-temperature/high-field NMR study we find an even more complex phase diagram close to the quasi-saturation field suggesting that bound two-magnon excitations are the lowest energy excitations close to and in the quasi-saturation regime. Qualitatively and semi-quantitatively, we relate such behavior to $XYZ$ exchange anisotropy and contributions from the Dzyaloshinsky-Moriya interaction to affect the magnetic properties of linarite.

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arXiv2018

MnSi-nanostructures obtained from thin films: magnetotransport and Hall effect

We present a comparative study of the (magneto)transport properties, including Hall effect, of bulk, thin film and nanostructured MnSi. In order to set our results in relation to published data we extensively characterize our materials, this way establishing a comparatively good sample quality. Our analysis reveals that in particular for thin film and nanostructured material, there are extrinsic and intrinsic contributions to the electronic transport properties, which by modeling the data we separate out. Finally, we discuss our Hall effect data of nanostructured MnSi under consideration of the extrinsic contributions and with respect to the question of the detection of a topological Hall effect in a skyrmionic phase.

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arXiv2017

Field induced Lifshitz transition in UPt$_2$Si$_2$: Fermi surface under extreme conditions

We have measured Hall effect, magnetotransport and magnetostriction on the field induced phases of single crystalline UPt$_2$Si$_2$ in magnetic fields up to 60\,T at temperatures down to 50\,mK. For the magnetic field applied along the $c$ axis we observe strong changes in the Hall effect at the phase boundaries. From a comparison to band structure calculations utilizing the concept of a dual nature of the uranium 5$f$ electrons, we find evidence for field induced topological changes of the Fermi surface due to at least one Lifshitz transition. Furthermore, we find a unique history dependence of the magnetotransport and magnetostriction data, indicating that the Lifshitz type transition is of a discontinuous nature, as predicted for interacting electron systems.

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arXiv2017

The dynamics of linarite: Observations of magnetic excitations

Here we present inelastic neutron scattering measurements from the frustrated, quantum spin-1/2 chain material linarite, PbCuSO_4(OH)_2. Time of flight data, taken at 0.5K and zero applied magnetic field reveals low-energy dispersive spin wave excitations below 1.5meV both parallel and perpendicular to the Cu-chain direction. From this we confirm that the interchain couplings within linarite are around 10% of the nearest neighbour intrachain interactions. We analyse the data within both linear spin-wave theory and density matrix renormalisation group theories and establish the main magnetic exchange interactions and the simplest realistic Hamiltonian for this material.

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arXiv2016

Electronic ground state of MnB$_{4}$

Recent studies have dealt with the electronic and magnetic ground state properties of the tetraboride material MnB$_4$. So far, however, the ground state properties could not be established unambiguously. Therefore, here we present an experimental study on single-crystalline MnB$_4$ by means of resistivity and magnetization measurements. For this, we have developed a sample holder that allows four-point ac resistivity measurements on these very small ($\sim$\,100\,$μ$m) samples. With our data we establish that the electronic ground state of MnB$_4$ is intrinsically that of a pseudo-gap system, in agreement with recent band structure calculations. Furthermore, we demonstrate that the material does neither show magnetic order nor a behavior arising from the vicinity to a magnetically ordered state, this way disproving previous claims.

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arXiv2015

Complex field-induced states in Linarite PbCuSO$_4$(OH)$_2$ with a variety of high-order exotic SDW$_p$ states

Low-temperature neutron diffraction and NMR studies of field-induced phases in linarite are presented for magnetic fields $H \parallel b$ axis. A two-step spin-flop transition is observed as well as a transition transforming a helical magnetic ground state into an unusual magnetic phase with sine-wave modulated moments $\parallel H$. An effective $\tilde{J}_1$-$\tilde{J}_2$ single-chain model with a magnetization-dependent frustration ratio $α_{\rm eff} = -\tilde{J}_2/\tilde{J}_1$ is proposed. The latter is governed by skew interchain couplings and shifted to the vicinity of the ferromagnetic critical point. It explains qualitatively the observation of a rich variety of exotic (for strongly correlated cuprate spin-1/2 Heisenberg systems) longitudinal collinear spin-density wave SDW$_p$ states ($9 \geq p \geq 2$).

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