arXiv subjects

H. C. Walker

Publications and source records attributed to H. C. Walker.

At least 19 recordsLinked to original sources

arXiv2025

Magnetic properties of the zigzag ladder compound SrTb2O4

We report on the properties of SrTb2O4, a frustrated zigzag ladder antiferromagnet, studied by single crystal neutron diffraction (with polarised neutrons in zero field and unpolarised neutrons in an applied magnetic field), as well as by neutron spectroscopy on a polycrystalline sample. The neutron scattering results are supported by single crystal magnetisation and heat capacity measurements. In zero field, neutron diffraction data show no transition to a magnetically ordered state down to the lowest experimentally available temperature of 35 mK, and the material remains magnetically disordered down to this temperature. Polarised neutron diffraction measurements reveal the presence of a diffuse scattering signal suggesting only very weak spin-spin correlations in the ground state. For H // c (the easy magnetisation direction), we followed the magnetisation process using neutron diffraction measurements and observed the appearance of field-induced magnetic Bragg peaks with integer h and k indices in the (hk0) scattering plane. No magnetic peaks with a non-zero propagation vector were detected. The observed in-field data fit well to a simple two-sublattice model with magnetic moments aligned along the field direction but being significantly different in magnitude for the two inequivalent Tb3+ sites in the unit cell. Overall, the collected data point to a nonmagnetic ground state in SrTb2O4 despite the presence of strong interactions.

cond-mat.str-el↗

arXiv2024

Anomalous quasielastic scattering contribution in the centrosymmetric multi-$\mathbf{q}$ helimagnet SrFeO$_3$

Centrosymmetric compounds which host three-dimensional topological spin structures comprise a distinct subclass of materials in which multiple-$\mathbf{q}$ magnetic order is stabilized by anisotropy and bond frustration in contrast to the more common path of antisymmetric exchange interactions. Here we investigate static and dynamic magnetic properties of the cubic perovskite SrFeO$_3$ $\unicode{x2013}$ a rare example of a centrosymmetric material hosting two types of topological spin textures: skyrmion- and hedgehog-lattice phases. Our detailed magnetization and dilatometry measurements describe the domain selection processes and phase transitions in SrFeO$_3$. Spin excitations are investigated using inelastic neutron scattering for all three zero-field phases. In the higher-temperature ordered phases, high-energy magnons increasingly lose coherence, so that spin fluctuations are dominated by a distinct quasielastic component at low energies. We anticipate that this could be generic to symmetric helimagnets in which the chiral symmetry is spontaneously broken by the magnetic order.

cond-mat.str-el↗

arXiv2022

Quantum critical spin-liquid-like behavior in S = 1/2 quasikagome lattice CeRh1-xPdxSn investigated using muon spin relaxation and neutron scattering

We present the results of muon spin relaxation ($μ$SR) and neutron scattering on the Ce-based quasikagome lattice CeRh$_{1-x}$Pd$_{x}$Sn ($x=0.1$ to 0.75). Our ZF-$μ$SR results reveal the absence of static long-range magnetic order down to 0.05~K in $x = 0.1$ single crystals. The weak temperature-dependent plateaus of the dynamic spin fluctuations below 0.2~K in ZF-$μ$SR together with its longitudinal-field (LF) dependence between 0 and 3~kG indicate the presence of dynamic spin fluctuations persisting even at $T$ = 0.05~K without static magnetic order. On the other hand, $C_{\text{4f}}$/$T$ increases as --log $T$ on cooling below 0.9~K, passes through a broad maximum at 0.13~K and slightly decreases on further cooling. The ac-susceptibility also exhibits a frequency independent broad peak at 0.16~K, which is prominent with an applied field $H$ along $c$-direction. We, therefore, argue that such a behavior for $x=0.1$ (namely, a plateau in spin relaxation rate ($λ$) below 0.2~K and a linear $T$ dependence in $C_{\text{4f}}$ below 0.13~K) can be attributed to a metallic spin-liquid (SL) ground state near the quantum critical point in the frustrated Kondo lattice. The LF-$μ$SR study suggests that the out of kagome plane spin fluctuations are responsible for the SL behavior. Low energy inelastic neutron scattering (INS) of $x$ = 0.1 reveals gapless magnetic excitations, which are also supported by the behavior of $C_{\text{4f}}$ proportional to $T^{1.1}$ down to 0.06~K.

cond-mat.str-el↗

arXiv2022

Valence bond glass state in the 4$d^1$ fcc antiferromagnet Ba$_2$LuMoO$_6$

$B$-site ordered 4$d^1$ and 5$d^1$ double perovskites have a number of potential novel ground states including multipolar order, quantum spin liquids and valence bond glass states. These arise from the complex interactions of spin-orbital entangled $J_{eff}$ = 3/2 pseudospins on the geometrically frustrated fcc lattice. The 4$d^1$ Mo$^{5+}$ perovskite Ba$_2$YMoO$_6$ has been suggested to have a valence bond glass ground state. Here we report on the low temperature properties of powder samples of isostructural Ba$_2$LuMoO$_6$: the only other known cubic 4$d^1$ perovskite with one magnetic cation. Our muon spectroscopy experiments show that magnetism in this material remains dynamic down to 60 mK without any spin freezing or magnetic order. A singlet-triplet excitation with a gap of $Δ$ = 28 meV is observed in inelastic neutron scattering. These results are interpreted as a disordered valence bond glass ground state similar to Ba$_2$YMoO$_6$. Our results highlight the differences of the 4$d^1$ double perovskites in comparison to cubic 5$d^1$ analogues, which have both magnetic and multipolar order.

cond-mat.str-el↗

arXiv2022

Frustration model and spin excitations in the helimagnet FeP

The metallic compound FeP belongs to the class of materials that feature a complex noncollinear spin order driven by magnetic frustration. While its double-helix magnetic structure with a period $λ_{\text{s}} \approx 5c$, where $c$ is the lattice constant, was previously well determined, the relevant spin-spin interactions that lead to that ground state remain unknown. By performing extensive inelastic neutron scattering measurements, we obtained the spin-excitation spectra in a large part of the momentum-energy space. The spectra show that the magnons are gapped with a gap energy of $\sim$5 meV. Despite the 3D crystal structure, the magnon modes display strongly anisotropic dispersions, revealing a quasi-one-dimensional character of the magnetic interactions in FeP. The physics of the material, however, is not determined by the dominating exchange, which is ferromagnetic. Instead, the weaker two-dimensional antiferromagnetic interactions between the rigid ferromagnetic spin chains drive the magnetic frustration. Using linear spin-wave theory, we were able to construct an effective Heisenberg Hamiltonian with an anisotropy term capable of reproducing the observed spectra. This enabled us to quantify the exchange interactions in FeP and determine the mechanism of its magnetic frustration.

cond-mat.str-el↗

arXiv2021

Magnetic order and crystalline electric field excitations of the quantum critical heavy fermion ferromagnet CeRh$_6$Ge$_4$

CeRh$_6$Ge$_4$ is an unusual example of a stoichiometric heavy fermion ferromagnet, which can be cleanly tuned by hydrostatic pressure to a quantum critical point. In order to understand the origin of this anomalous behavior, we have characterized the magnetic ordering and crystalline electric field (CEF) scheme of this system. While magnetic Bragg peaks are not resolved in neutron powder diffraction, coherent oscillations are observed in zero-field $μ$SR below $T_{\rm C}$, which are consistent with in-plane ferromagnetic ordering consisting of reduced Ce moments. From analyzing the magnetic susceptibility and inelastic neutron scattering, we propose a CEF-level scheme which accounts for the easy-plane magnetocrystalline anisotropy, where the low lying first excited CEF exhibits significantly stronger hybridization than the ground state. These results suggest that the orbital anisotropy of the ground state and low lying excited state doublets are important for realizing anisotropic electronic coupling between the $f$- and conduction electrons, which gives rise to the highly anisotropic hybridization observed in photoemission experiments.

cond-mat.str-el↗

arXiv2021

Metastable antiphase boundary ordering in CaFe$_{2}$O$_{4}$

CaFe$_{2}$O$_{4}$ is an $S=5/2$ antiferromagnet exhibiting two magnetic orders which shows regions of coexistence at some temperatures. Using a Green's function formalism, we model neutron scattering data of the spin wave excitations in this material, ellucidating the microscopic spin Hamiltonian. In doing so, we suggest that the low temperature A phase order $(\uparrow\uparrow\downarrow\downarrow)$ finds its origins in the freezing of antiphase boundaries created by thermal fluctuations in a parent B phase order $(\uparrow\downarrow\uparrow\downarrow)$. The low temperature magnetic order observed in CaFe$_{2}$O$_{4}$ is thus the result of a competition between the exchange coupling along $c$, which favors the B phase, and the single-ion anisotropy which stabilizes thermally-generated antiphase boundaries, leading to static metastable A phase order at low temperatures.

cond-mat.str-el↗

arXiv2021

Magnetic correlations in triangular antiferromagnet FeGa$_2$S$_4$

The crystal structure and magnetic correlations in triangular antiferromagnet FeGa$_2$S$_4$ are studied by x-ray diffraction, magnetic susceptibility, neutron diffraction and neutron inelastic scattering. We report significant mixing at the cation sites and disentangle magnetic properties dominated by major and minor magnetic sites. The magnetic short-range correlations at 0.77 Å$^{-1}$ correspond to the major sites and being static at base temperature they evolve into dynamic correlations around 30 - 50 K. The minor sites contribute to the magnetic peak at 0.6 Å$^{-1}$, which vanishes at 5.5 K. Our analytical studies of triangular lattice models with bilinear and biquadratic terms provide the ratios between exchanges for the proposed ordering vectors. The modelling of the inelastic neutron spectrum within linear spin wave theory results in the set of exchange couplings $J_1=1.7$\,meV, $J_2=0.9$\,meV, $J_3=0.8$\,meV for the bilinear Heisenberg Hamiltonian. However, not all features of the excitation spectrum are explained with this model.

cond-mat.str-el↗

arXiv2021

Order-by-Disorder from Bond-Dependent Exchange and Intensity Signature of Nodal Quasiparticles in a Honeycomb Cobaltate

Recent theoretical proposals have argued that cobaltates with edge-sharing octahedral coordination can have significant bond-dependent exchange couplings thus offering a platform in 3$d$ ions for such physics beyond the much-explored realizations in 4$d$ and 5$d$ materials. Here we present high-resolution inelastic neutron scattering data within the magnetically ordered phase of the stacked honeycomb magnet CoTiO$_3$ revealing the presence of a finite energy gap and demonstrate that this implies the presence of bond-dependent anisotropic couplings. We also show through an extensive theoretical analysis that the gap further implies the existence of a quantum order-by-disorder mechanism that, in this material, crucially involves virtual crystal field fluctuations. Our data also provide an experimental observation of a universal winding of the scattering intensity in angular scans around linear band-touching points for both magnons and dispersive spin-orbit excitons, which is directly related to the non-trivial topology of the quasiparticle wavefunction in momentum space near nodal points.

cond-mat.str-el↗

arXiv2021

A crossover from Kondo semiconductor to metallic antiferromagnet with $5d$-electron doping in CeFe$_2$Al$_{10}$

We report a systematic study of the $5d$-electron-doped system Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$ ($0 \leq x \leq 0.15$). With increasing $x$, the orthorhombic $b$~axis decreases slightly while accompanying changes in $a$ and $c$ leave the unit cell volume almost unchanged. Inelastic neutron scattering, along with thermal and transport measurements, reveal that for the Kondo semiconductor CeFe$_2$Al$_{10}$, the low-temperature energy gap which is proposed to be a consequence of strong $c \mhyphen f$ hybridization, is suppressed by a small amount of Ir substitution for Fe, and that the system adopts a metallic ground state with an increase in the density of states at the Fermi level. The charge or transport gap collapses (at $x=$~0.04) faster than the spin gap with Ir substitution. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements demonstrate that the system undergoes long-range antiferromagnetic order below a Néel temperature, $T_{\mathrm{N}}$, of 3.1(2)~K for $x = 0.15$. The ordered moment is estimated to be smaller than 0.07(1)~$μ_\mathrm{B}$/Ce although the trivalent state of Ce is confirmed by Ce L$_3$-edge x-ray absorption near edge spectroscopy. It is suggested that the $c \mhyphen f$ hybridization gap, which plays an important role in the unusually high ordering temperatures observed in Ce$T_2$Al$_{10}$ ($T$ = Ru and Os), may not be necessary for the onset of magnetic order with a low $T_{\mathrm{N}}$ seen here in Ce(Fe$_{1-x}$Ir$_x$)$_2$Al$_{10}$.

cond-mat.str-el↗

arXiv2021

From one- to two-magnon excitations in the S=3/2 magnet $β$-CaCr$_2$O$_4$

We apply neutron spectroscopy to measure the magnetic dynamics in the S=3/2 magnet $β$-CaCr$_2$O$_4$ (T$_N$=21 K). The low-energy fluctuations, in the ordered state, resemble large-S linear spin-waves from the incommensurate ground state. However, at higher energy transfers, these semi-classical and harmonic dynamics are replaced by an energy and momentum broadened continuum of excitations. Applying kinematic constraints required for energy and momentum conservation, sum rules of neutron scattering, and comparison against exact diagonalization calculations, we show that the dynamics at high-energy transfers resemble low-S one-dimensional quantum fluctuations. $β$-CaCr$_2$O$_4$ represents an example of a magnet at the border between classical Néel and quantum phases, displaying dual characteristics.

cond-mat.str-el↗

arXiv2020

Lattice dynamics in the double-helix antiferromagnet FeP

We present a comprehensive investigation of lattice dynamics in the double-helix antiferromagnet FeP by means of high-resolution time-of-flight neutron spectroscopy and ab-initio calculations. Phonons can hybridize with the magnetic excitations in noncollinear magnets to significantly influence their properties. We observed a rich spectrum of phonon excitations, which extends up to $\sim$50 meV. We performed detailed analysis of the observed and calculated spectra for all high-symmetry points and high-symmetry directions of the Brillouin zone. We show that the DFT calculations quantitatively capture the essential features of the observed phonons, including both dispersions and scattering intensities. By making use of the detailed intensity comparison between the theory and the data, we were able to identify displacement vectors for the majority of the observed modes. The overall excellent agreement between the DFT predictions and the experimental results breaks down for the lowest mode at the $Y$-point, whose energy is lower than calculated by $\sim$13%. The present study provides vital information on the lattice dynamics in FeP and demonstrates applicability of the DFT to novel pressure-induced phenomena in related materials, such as MnP and CrAs.

cond-mat.str-el↗

arXiv2020

Orbital-selective spin waves in detwinned NaFeAs

The existence of orbital-dependent electronic correlations has been recognized as an essential ingredient to describe the physics of iron-based superconductors. NaFeAs, a parent compound of iron based superconductors, exhibits a tetragonal-to-orthorhombic lattice distortion below $T_s\approx 60$ K, forming an electronic nematic phase with two 90$^\circ$ rotated (twinned) domains, and orders antiferromagnetically below $T_N\approx 42$ K. We use inelastic neutron scattering to study spin waves in uniaxial pressure-detwinned NaFeAs. By comparing the data with combined density functional theory and dynamical mean-field theory calculations, we conclude that spin waves up to an energy scale of $E_\text{crossover} \approx 100$ meV are dominated by $d_{yz}$-$d_{yz}$ intra-orbital scattering processes, which have the two-fold ($C_2$) rotational symmetry of the underlying lattice. On the other hand, the spin wave excitations above $E_\text{crossover}$, which have approximately fourfold ($C_4$) rotational symmetry, arise from the $d_{xy}$-$d_{xy}$ intra-orbital scattering that controls the overall magnetic bandwidth in this material. In addition, we find that the low-energy ($E\approx 6$ meV) spin excitations change from approximate $C_4$ to $C_2$ rotational symmetry below a temperature $T^\ast$ ($>T_s$), while spin excitations at energies above $E_\text{crossover}$ have approximate $C_4$ rotational symmetry and are weakly temperature dependent. These results are consistent with angle resolved photoemission spectroscopy measurements, where the presence of an uniaxial strain necessary to detwin NaFeAs also raises the onset temperature $T^\ast$ of observable orbital-dependent band splitting to above $T_s$, thus supporting the notion of orbital selective spin waves in the nematic phase of iron-based superconductors.

cond-mat.supr-con↗

arXiv2020

Long-range magnetic order in the ${\tilde S}=1/2$ triangular lattice antiferromagnet KCeS$_2$

Recently, several putative quantum spin liquid (QSL) states were discovered in ${\tilde S} = 1/2$ rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS$_2$ and show via low-temperature specific heat and $μ$SR investigations that it yields magnetic order below $T_{\mathrm N} = 0.38$ K despite the same delafossite structure. We identify a well separated ${\tilde S} = 1/2$ ground state for KCeS$_2$ from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane $g$~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS$_2$.

cond-mat.str-el↗

arXiv2020

Charge disproportionation and nano phase separation in $R$SrNiO$_4$

We have successfully grown centimeter-sized layered $R$SrNiO$_4$ single crystals under high oxygen pressures of 120 bar by the floating zone technique. This enabled us to perform neutron scattering experiments where we observe close to quarter-integer magnetic peaks below $\sim$77 K that are accompanied by steep upwards dispersing spin excitations. Within the high-frequency Ni-O bond stretching phonon dispersion, a softening at the propagation vector for a checkerboard modulation can be observed. Together with our spin wave simulations these observations reveal that this Ni$^{3+}$ system exhibits charge disproportionation with charges segregating into a checkerboard pattern within a nano phase separation scenario rather than showing a Jahn-Teller effect.

cond-mat.str-el↗

arXiv2020

Evidence for biquadratic exchange in the quasi-two-dimensional antiferromagnet FePS$_3$

FePS$_3$ is a van der Waals compound with a honeycomb lattice that is a good example of a two-dimensional antiferromagnet with Ising-like anisotropy. Neutron spectroscopy data from FePS3 were previously analysed using a straight-forward Heisenberg Hamiltonian with a single-ion anisotropy. The analysis captured most of the elements of the data, however some significant discrepancies remained. The discrepancies were most obvious at the Brillouin zone boundaries. The data are subsequently reanalysed allowing for unequal exchange between nominally equivalent nearest-neighbours, which resolves the discrepancies. The source of the unequal exchange is attributed to a biquadratic exchange term in the Hamiltonian which most probably arises from a strong magnetolattice coupling. The new parameters show that there are features consistent with Dirac magnon nodal lines along certain Brillouin zone boundaries.

cond-mat.mtrl-sci↗

arXiv2020

Exchange Interactions Mediated by Non-Magnetic Cations in Double Perovskites

Establishing the physical mechanism governing exchange interactions is fundamental for exploring exotic phases such as the quantum spin liquids (QSLs) in real materials. In this work, we address exchange interactions in Sr2CuTe$_{1-x}$W$_{x}$O, a series of double perovskites that realize the spin-1/2 square lattice and were suggested to harbor a QSL ground state arising from random distribution of non-magnetic ions. Our {\it ab initio} multi-reference configuration interaction calculations show that replacing Te atoms with W atoms changes the dominant couplings from nearest to next-nearest neighbor explained by the crucial role of unoccupied states of non-magnetic ions in the super-superexchange mechanism. Combined with spin-wave theory simulations, our calculated exchange couplings provide an excellent description of the inelastic neutron scattering spectra of the end compounds, as well as explain the magnetic excitations in Sr2CuTe$_{0.5}$W$_{0.5}$O as emerging from the bond-disordered exchange couplings. Our results provide crucial understanding of the role of non-magnetic cations in exchange interactions paving the way to further exploration of QSL phases in bond-disordered materials.

cond-mat.str-el↗

arXiv2019

Spin fluctuation anisotropy as a probe of orbital-selective hole-electron quasiparticle excitations in detwinned Ba(Fe1-xCox)2As2

We use inelastic neutron scattering to study spin excitation anisotropy in mechanically detwinned Ba(Fe1-xCox)2As2 with x = 0.048 and 0.054. Both samples exhibit a tetragonal-to-orthorhombic structural transition at Ts, a collinear static antiferromagnetic (AF) order at wave vector Q1 = QAF = (1, 0) below the Neel temperature TN, and superconductivity below Tc (Ts > TN > Tc). In the high temperature paramagnetic tetragonal phase (T > Ts), spin excitations centered at Q1 and Q2 = (0, 1) are gapless and have four-fold (C4) rotational symmetry. On cooling to below TN but above Tc, spin excitations become highly anisotropic, developing a gap at Q2 but still are gapless at Q1. Upon entering into the superconducting state, a neutron spin resonance appears at Q1 with no magnetic scattering at Q2. By comparing these results with those from angle resolved photoemission spectroscopy experiments, we conclude that the anisotropic shift of the dyz and dxz bands in detwinned Ba(Fe1-xCox)2As2 below Ts is associated with the spin excitation anisotropy, and the superconductivity-induced resonance arises from the electron-hole Fermi surface nesting of quasiparticles with the dyz orbital characters.

cond-mat.supr-con↗