arXiv subjects

M. Reehuis

Publications and source records attributed to M. Reehuis.

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.

cond-mat.str-el↗

arXiv2023

The crystal and magnetic structure of cesium superoxide

CsO2 is a member of the family of alkali superoxides (formula AO2 with A= Na, K, Rb and Cs) that exhibit magnetic behavior arising from open $p$-shell electrons residing on O2- molecules. We use neutron diffraction to solve the crystal and magnetic structures of CsO2, and observe a complex series of structures on cooling from room temperature to 1.6 K. These include an incommensurate modulation along the a-axis of the structure at intermediate temperatures, which then locks into a commensurate modulation that doubles the unit cell compared to the previously supposed orthorhombic unit cell. In both incommensurate and commensurate phases our structural solution involves a staggering of the cesium ion positions along the b-axis, in contrast to studies of other alkali superoxides in which staggered tilts of the O2- dimers relative to the c-axis are seen. Below T ~ 10 K we observe magnetic Bragg reflections arising from an antiferromagnetically ordered structure with a wavevector of k = (0,0,0) (relative to the doubled crystallographic unit cell), with moments that point predominantly along the b-axis with a small component along the a-axis that hints at possible anisotropic exchange coupling (consistent with the crystal structure). Measurements of the magnetic Bragg reflections in an applied magnetic field suggest a spin-flop transition takes place between 2 T and 4 T in which moments likely flop to point along the crystallographic a-axis. Our measurements indicate that CsO2 is an interesting example of magnetic properties being inherently linked to the crystal structure, in that the staggered displacement of the cesium ions activates antisymmetric exchange which then permits the observed spin canting.

cond-mat.str-el↗

arXiv2023

Magnetic-field induced melting of long-range magnetic order akin to Kitaev insulators in the metallic compound Tb5Si3

There have been constant efforts to find exotic quantum spin-liquid (QSL) materials. Some of the transition metal insulators dominated by the direction dependent anisotropic exchange interaction (Kitaev model for honeycomb network of magnetic ions) are considered to be promising cases for the same. In such Kitaev insulators, QSL is achieved from the zero-field antiferromagnetic state by the application of magnetic field, suppressing other exchange interactions responsible for magnetic order. Here, we show that the features attributable to long-range magnetic ordering of the intermetallic compound, Tb5Si3 (T_N= 69 K), containing honey-comb network of Tb ions, are completely suppressed by a critical applied field, H_cr, in heat-capacity and magnetization data, mimicking the behavior of Kitaev physics candidates. The neutron diffraction patterns as a function of H reveal that it is an incommensurate magnetic structure that gets suppressed, showing peaks arising from multiple wave vectors beyond Hcr. Increasing magnetic entropy as a function of H with a peak in the magnetically ordered state is in support of some kind of magnetic disorder in a narrow field range after H_cr. Such a high-field behavior for a metallic heavy rare-earth system to our knowledge has not been reported in the past and therefore is intriguing.

cond-mat.str-el↗

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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2020

Neutron Diffraction Evidence for Local Spin Canting, Weak Jahn-Teller Distortion, and Magnetic Compensation in Ti$_{1-x}$Mn$_{x}$Co$_2$O$_4$ Spinel

A systematic study using neutron diffraction and magnetic susceptibility are reported on Mn substituted ferrimagnetic inverse spinel Ti$_{1-x}$Mn$_{x}$Co$_2$O$_4$ in the temperature interval 1.6 K $\leq$ $T$ $\leq$ 300 K. Our neutron diffraction study reveals cooperative distortions of the $T$O$_6$ octahedral for all the Jahn-Teller active ions $T$ = Mn$^{3+}$, Ti$^{3+}$ and Co$^{3+}$, which are confirmed by the X-ray photoelectron spectroscopy. Two specific compositions ($x$ = 0.2 and 0.4) have been chosen because of their unique features: noncollinear Yafet-Kittel type ordering, and weak tetragonal distortion with ${c/a}$ $<$ 1, in which the apical bond length $d_c$($T_B$-O) is longer than the equatorial $d_{ab}$($T_B$-O) due to the splitting of the $e_g$ level of Mn$^{3+}$ ions into $d_{x^2-y^2}$ and $d_{z^2}$. For $x$ = 0.4, the distortion in the $T_B$O$_6$ octahedra is stronger as compared to $x$ = 0.2 because of the higher content of trivalent Mn. Ferrimagnetic ordering in $x$ = 0.4 and $x$ = 0.2 sets in at 110.3 and 78.2 K, respectively due to the unequal magnetic moments of cations, where Ti$^{3+}$, Mn$^{3+}$, and Co$^{3+}$ occupying the octahedral, whereas, Co$^{2+}$ sits in the tetrahedral site. In addition, weak antiferromagnetic component could be observed lying perpendicular to the ferrimagnetic component. The analysis of static and dynamic magnetic susceptibilities combined with the heat-capacity data reveals a magnetic compensation phenomenon at $T_{COMP}$ = 25.4 K in $x$ = 0.2 and a reentrant spin-glass behaviour in $x$ = 0.4 with a freezing temperature $\sim$110.1 K. The compensation phenomenon is characterized by sign reversal of magnetization and bipolar exchange bias effect below $T_{COMP}$ with its magnitude depending on the direction of external magnetic field and the cooling protocol.

cond-mat.str-el↗

arXiv2019

Spin-dimer ground state driven by consecutive charge and orbital ordering transitions in the anionic mixed-valence compound Rb$_4$O$_6$

Recently, a Verwey-type transition in the mixed-valence alkali sesquioxide Cs$_4$O$_6$ was deduced from the charge ordering of molecular peroxide O$_2^{2-}$ and superoxide O$_2^-$ anions accompanied by the structural transformation and a dramatic change in electronic conductivity [Adler et al, Sci. Adv 4, eaap7581 (2018)]. Here, we report that in the sister compound Rb$_4$O$_6$ a similar Verwey-type charge ordering transition is strongly linked to O$_2^-$ orbital and spin dynamics. On cooling, a powder neutron diffraction experiment reveals a charge ordering and a cubic-to-tetragonal transition at $T_{\rm CO}=290$ K, which is followed by a further structural instability at $T_{\rm s}=92$ K that involves an additional reorientation of magnetic O$_2^-$ anions. Magnetic resonance techniques supported by density functional theory computations suggest the emergence of a peculiar type of $π^*$-orbital ordering of the magnetically active O$_2^-$ units, which promotes the formation of a quantum spin state composed of weakly coupled spin dimers. These results reveal that similarly as in 3$d$ transition metal compounds, also in in the $π^*$ open-shell alkali sesquioxides the interplay between Jahn-Teller-like electron-lattice coupling and Kugel-Khomskii-type superexchange determines the nature of orbital ordering and the magnetic ground state.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2016

Electronic properties of a heavy-fermion U(Ru0.92Rh0.08)2Si2 single crystal

We report the crystal structure and highly-anisotropic magnetic, transport and thermal properties of an exceptionally good single crystal of U(Ru0.92Rh0.08)2Si2 prepared using a modified Czochralski method. Our study, that also includes neutron diffraction results, shows all the heavy-fermion signatures of pristine URu2Si2 , however, the superconductivity, hidden order and remanent weak antiferromagnetic orders are absent. Instead, the ground state of the doped system can be classified as a spin liquid that preserves the heavy-fermion character. U(Ru0.92Rh0.08)2Si2 exhibits a short-range magnetic order distinguished by reflections of a Lorentzian profile at qIII = (1/2 1/2 1/2) positions that disappear above approx. 15 K. The short-range order seems to be a precursor of a long-range magnetic order that occurs with higher Rh concentration. We indicate that these short-range fluctuations involve, at least partially, inelastic scattering processes.

cond-mat.str-el↗

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 ($9 \geq p \geq 2$).

cond-mat.str-el↗

arXiv2015

Jahn-Teller versus quantum effects in the spin-orbital material LuVO3

We report on combined neutron and resonant x-ray scattering results, identifying the nature of the spin-orbital ground state and magnetic excitations in LuVO3 as driven by the orbital parameter. In particular, we distinguish between models based on orbital Peierls dimerization, taken as a signature of quantum effects in orbitals, and Jahn-Teller distortions, in favor of the latter. In order to solve this long-standing puzzle, polarized neutron beams were employed as a prerequisite in order to solve details of the magnetic structure, which allowed quantitative intensity-analysis of extended magnetic excitation data sets. The results of this detailed study enabled us to draw definite conclusions about classical vs quantum behavior of orbitals in this system and to discard the previous claims about quantum effects dominating the orbital physics of LuVO3 and similar systems.

cond-mat.str-el↗

arXiv2015

An orbital glass state of a nearly metallic spinel, CoV$_2$O$_4$

Strain, magnetization, and unpolarized and polarized neutron diffraction measurements were performed to study the magnetic and structural properties of spinel CoV$_{2}$O$_{4}$. Magnetostriction measurements indicate that a subtle distortion of the crystal along the direction of magnetization, $ΔL/L \sim 10^{-4}$, exists and varies from elongation to contraction in a second order fashion upon cooling. Unpolarized and polarized single-crystal neutron experiments indicate that upon cooling the ferrimagnetic structure changes from collinear to noncollinear at $T \sim 90$ K, where the elongation of the crystal is maximized. These results imply the existence of an orbital glassy state in the nearly metallic frustrated magnet CoV$_{2}$O$_{4}$.

cond-mat.str-el↗

arXiv2014

FeCr$_2$S$_4$ in magnetic fields: possible evidence for a multiferroic ground state

We report on neutron diffraction, thermal expansion, magnetostriction, dielectric, and specific heat measurements on polycrystalline FeCr2S4 in external magnetic fields. The ferrimagnetic ordering temperatures $T_{\mathrm{C}}\approx 170$ K and the transition at $T_{\mathrm{OO}}\approx 10$ K, which has been associated with orbital ordering, are only weakly shifted in magnetic fields up to 9 T. The cubic lattice parameter is found to decrease when entering the state below $T_{\mathrm{OO}}$. The magnetic moments of the Cr- and Fe-ions are reduced from the spin-only values throughout the magnetically ordered regime, but approach the spin-only values for fields $>$5.5 T. Thermal expansion in magnetic fields and magnetostriction experiments indicate a contraction of the sample below about 60 K. Below $T_{\mathrm{OO}}$ this contraction is followed by a moderate expansion of the sample for fields larger than $\sim$4.5 T. The transition at $T_{\mathrm{OO}}$ is accompanied by an anomaly in the dielectric constant. The dielectric constant depends on both the strength and orientation of the external magnetic field with respect to the applied electric field for $T<T_{\mathrm{OO}}$. A linear correlation of the magnetic-field-induced change of the dielectric constant and the magnetic-field dependent magnetization is observed. This behaviour is consistent with the existence of a ferroelectric polarization and a multiferroic ground state below 10 K.

cond-mat.str-el↗

arXiv2014

Competing exchange interactions on the verge of a metal-insulator transition in the two-dimensional spiral magnet Sr$_3$Fe$_2$O$_7$

We report a neutron scattering study of the magnetic order and dynamics of the bilayer perovskite Sr$_3$Fe$_2$O$_7$, which exhibits a temperature-driven metal-insulator transition at 340 K. We show that the Fe$^{4+}$ moments adopt incommensurate spiral order below $T_\text{N}=115$ K and provide a comprehensive description of the corresponding spin wave excitations. The observed magnetic order and excitation spectra can be well understood in terms of an effective spin Hamiltonian with interactions ranging up to third nearest-neighbor pairs. The results indicate that the helical magnetism in Sr$_3$Fe$_2$O$_7$ results from competition between ferromagnetic double-exchange and antiferromagnetic superexchange interactions whose strengths become comparable near the metal-insulator transition. They thus confirm a decades-old theoretical prediction and provide a firm experimental basis for models of magnetic correlations in strongly correlated metals.

cond-mat.str-el↗

arXiv2013

Thermodynamic Properties of the Anisotropic Frustrated Spin-chain Compound Linarite PbCuSO$_4$(OH)$_2$

We present a comprehensive macroscopic thermodynamic study of the quasi-one-dimensional (1D) $s = \tfrac{1}{2}$ frustrated spin-chain system linarite. Susceptibility, magnetization, specific heat, magnetocaloric effect, magnetostriction, and thermal-expansion measurements were performed to characterize the magnetic phase diagram. In particular, for magnetic fields along the b axis five different magnetic regions have been detected, some of them exhibiting short-range-order effects. The experimental magnetic entropy and magnetization are compared to a theoretical modelling of these quantities using DMRG and TMRG approaches. Within the framework of a purely 1D isotropic model Hamiltonian, only a qualitative agreement between theory and the experimental data can be achieved. Instead, it is demonstrated that a significant symmetric anisotropic exchange of about 10% is necessary to account for the basic experimental observations, including the 3D saturation field, and which in turn might stabilize a triatic (three-magnon) multipolar phase.

cond-mat.str-el↗

arXiv2013

Magnetic phase diagram of $Sr_3 Fe_2 O_{7-x}$

Magnetometry, electrical transport, and neutron scattering measurements were performed on single crystals of the Fe^{4+}-containing perovskite-related phase Sr_3Fe_2O_7-x as a function of oxygen content. Although both the crystal structure and electron configuration of this compound are closely similar to those of well-studied ruthenates and manganates, it exhibits very different physical properties. The fully-oxygenated compound (x=0) exhibits a charge-disproportionation transition at T_D = 340 K, and an antiferromagnetic transition at T_N = 115 K. For temperatures T \leq T_D, the material is a small-gap insulator; the antiferromagnetic order is incommensurate, which implies competing exchange interactions between the Fe^{4+} moments. The fully-deoxygenated compound (x=1) is highly insulating, and its Fe^{3+} moments exhibit commensurate antiferromagnetic order below T_N ~ 600 K. Compounds with intermediate x exhibit different order with lower T_N, likely as a consequence of frustrated exchange interactions between Fe^{3+} and Fe^{4+} sublattices. A previous proposal that the magnetic transition temperature reaches zero is not supported.

cond-mat.str-el↗

arXiv2012

Floating Zone Growth of Large Single Crystals of SrFeO_3-x

The Fe^{4+}-containing cubic perovskite phase SrFeO_3-x is of interest both for its high-temperature, oxygen-conducting properties as a solid oxide fuel cell component, and at low temperatures, where it exhibits a plethora of helical magnetic phases and a candidate Skyrmion lattice. However, a sequence of structural phase transitions encountered on cooling to room temperature has limited the size of single crystals. We report the floating-zone growth and oxygen-annealing of multiple-cubic-centimetre-sized single crystals of SrFeO_3-x, suitable for inelastic neutron scattering and other measurement techniques requiring large sample volumes.

cond-mat.mtrl-sci↗

arXiv2012

Neutron diffraction study of spin and charge ordering in SrFeO(3-delta)

We report a comprehensive neutron diffraction study of the crystal structure and magnetic order in a series of single-crystal and powder samples of SrFeO$_{3-δ}$ in the vacancy range $0 \leq δ\leq 0.23$. The data provide detailed insights into the interplay between the oxygen vacancy order and the magnetic structure of this system. In particular, a crystallographic analysis of data on Sr8Fe8O23 revealed a structural transition between the high-temperature tetragonal and a low-temperature monoclinic phase with a critical temperature T = 75 K, which originates from charge ordering on the Fe sublattice and is associated with a metal-insulator transition. Our experiments also revealed a total of seven different magnetic structures of SrFeO$_{3-δ}$ in this range of $δ$, only two of which (namely an incommensurate helix state in SrFeO3 and a commensurate, collinear antiferromagnetic state in Sr4Fe4O11) had been identified previously. We present a detailed refinement of some of the magnetic ordering patterns and discuss the relationship between the magneto-transport properties of SrFeO$_{3-δ}$ samples and their phase composition and magnetic microstructure.

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