arXiv subjects

S. J. Clark

Publications and source records attributed to S. J. Clark.

At least 19 recordsLinked to original sources

arXiv2026

Local magnetic properties of the rare-earth intermetallics $R$Mn$_2$Ge$_2$ ($R$=Ce, Pr, Nd)

We present an investigation of the rare-earth intermetallic materials, $R$Mn$_2$Ge$_2$ ($R$=Ce, Pr, Nd), reported to host a lattice of skyrmionic bubbles at room temperature. The magnetism of all three materials is characterised by the onset of local fluctuations as the magnetic state changes from a conical magnetic structure to a collinear antiferromagnetic one as temperature $T$ is increased. In this $T$ regime, where skyrmion-bubble textures have been reported, we see dynamics similar to those observed in other skyrmion-hosting materials. The level of disorder above this transition increases across the series from $R$=Ce to Nd. At low temperatures the magnetism is affected by the ordering of the rare-earth ions, resulting in distinct behaviour for the different members of the series.

cond-mat.str-el↗

arXiv2025

Heterometallic spin-1/2 quantum magnet under hydrostatic pressure

We investigate the properties of CuVOF$_4$(H$_2$O)$_6$$\cdot$H$_2$O, in which two different spin species, Cu(II) and V(IV), form antiferromagnetic spin-1/2 dimers with weak interdimer coupling provided via hydrogen bonding. Using radio-frequency susceptometry and electron-spin resonance (ESR), we show how the temperature-magnetic field spin-dimer phase diagram evolves as a function of applied hydrostatic pressure and correlate this with pressure-induced changes to the crystal structure. These results, coupled with pressure-tuned DFT calculations, confirm the prior prediction that the primary exchange interaction is mediated via an unusual mechanism in which the V(IV) ions provide considerable spin density to the oxygen that joins the two spins in each dimer and which lies along the Jahn-Teller axis of the Cu(II) ion. In addition, the dissimilarity in the spins that make up each dimer unit leads to a non-linear field dependence of the electronic energy levels as detected in the ESR measurements.

cond-mat.str-el↗

arXiv2025

Magnetism in $M_{1/3}$NbS$_2$ ($M$ = Fe, V, Mn): insight into intercalated transition-metal dichalcogenides using $\mu$SR

We present the results of muon-spin relaxation ($\mu$SR) measurements of the static and dynamic magnetism of $M_{1/3}$NbS$_2$ ($M$ = Fe, V, Mn), three intercalated transition-metal dichalcogenides. Transitions to long-range magnetic order are observed in all three materials and local magnetic fields at muon sites are compared to dipole field calculations. Measurements on Fe$_{1/3}$NbS$_2$ capture the evolution of two coexisting magnetic phases. In V$_{1/3}$NbS$_2$ we observe a peak in the dynamic response at $9$ K, coincident with previous reports of a possible low-temperature phase transition. The observation of high-frequency muon precession in Mn$_{1/3}$NbS$_2$ suggests the existence of an additional muon site that implies a difference in electronic energy landscape compared to the other materials in the series. Taken together, this demonstrates that the change in intercalant species drives significant variations in magnetism, highlighting the $M_{1/3}$NbS$_2$ ($M$ = Fe, V, Mn) series as an ideal group of materials for investigating a wide range of magnetic phenomena.

cond-mat.str-el↗

arXiv2025

Anisotropic skyrmion and multi-$q$ spin dynamics in centrosymmetric Gd$_2$PdSi$_3$

Skyrmions are particle-like vortices of magnetization with non-trivial topology, which are usually stabilized by Dzyaloshinskii-Moriya interactions (DMI) in noncentrosymmetric bulk materials. Exceptions are centrosymmetric Gd- and Eu-based skyrmion-lattice (SkL) hosts with zero DMI, where both the SkL stabilization mechanisms and magnetic ground states remain controversial. We address these here by investigating both the static and dynamical spin properties of the centrosymmetric SkL host Gd$_2$PdSi$_3$ using muon spectroscopy ($μ$SR). We find that spin fluctuations in the non-coplanar SkL phase are highly anisotropic, implying that spin anisotropy plays a prominent role in stabilizing this phase. We also observe strongly-anisotropic spin dynamics in the ground-state (IC-1) incommensurate magnetic phase of the material, indicating that it hosts a meron-like multi-$q$ structure. In contrast, the higher-field, coplanar IC-2 phase is found to be single-$q$ with nearly-isotropic spin dynamics.

cond-mat.str-el↗

arXiv2025

Muon spectroscopy investigation of anomalous dynamic magnetism in NiI$_2$

We present the results of muon-spin relaxation ($μ^{+}$SR) measurements of the van der Waals magnet NiI$_2$, which probe magnetic phase transitions at $T_{\mathrm{N1}}=73$~K and $T_{\mathrm{N2}}=60$~K. Supporting density functional theory (DFT) calculations allow the determination of a single muon stopping site whose magnetic environment is consistent with the proposed ground-state magnetic structure. $μ^{+}$SR measurements of the dynamics reveal behavior consistent with spin-wave excitations below $T_{\mathrm{N2}}$. In the region $T_{\mathrm{N2}}<T<T_{\mathrm{N1}}$ the character of the dynamics changes qualitatively, resulting in an unusual region of temperature-independent fluctuations.

cond-mat.str-el↗

arXiv2023

Asymmetric phase diagram and dimensional crossover in a system of spin-1/2 dimers under applied hydrostatic pressure

We present the magnetic and structural properties of [Cu(pyrazine)$_{0.5}$(glycine)]ClO$_4$ under applied pressure. As previously reported, at ambient pressure this material consists of quasi-two-dimensional layers of weakly coupled antiferromagnetic dimers which undergo Bose-Einstein condensation of triplet excitations between two magnetic field-induced quantum critical points (QCPs). The molecular building blocks from which the compound is constructed give rise to exchange strengths that are considerably lower than those found in other $S = 1/2$ dimer materials, which allows us to determine the pressure evolution of the entire field-temperature magnetic phase diagram using radio-frequency magnetometry. We find that a distinct phase emerges above the upper field-induced transition at elevated pressures and also show that an additional QCP is induced at zero-field at a critical pressure of $p_{\rm c} = 15.7(5)$ kbar. Pressure-dependent single-crystal X-ray diffraction and density functional theory calculations indicate that this QCP arises primarily from a dimensional crossover driven by an increase in the interdimer interactions between the planes. While the effect of quantum fluctuations on the lower field-induced transition is enhanced with applied pressure, quantum Monte Carlo calculations suggest that this alone cannot explain an unconventional asymmetry that develops in the phase diagram.

cond-mat.str-el↗

arXiv2023

Many-Body Quantum Muon Effects and Quadrupolar Coupling in Solids

Strong quantum zero-point motion (ZPM) of light nuclei and other particles is a crucial aspect of many state-of-the-art quantum materials. However, it has only recently begun to be explored from an $\textit{ab initio}$ perspective, through several competing approximations. Here we develop a unified description of muon and light nucleus ZPM and establish the regimes of anharmonicity and positional quantum entanglement where different approximation schemes apply. Via density functional theory and path-integral molecular dynamics simulations we demonstrate that in solid nitrogen, $α\unicode{x2013}$N$_2$, muon ZPM is both strongly anharmonic and many-body in character, with the muon forming an extended electric-dipole polaron around a central, quantum-entangled [N$_2\unicode{x2013}μ\unicode{x2013}$N$_2$]$^+$ complex. By combining this quantitative description of quantum muon ZPM with precision muon quadrupolar level-crossing resonance experiments, we independently determine the static $^{14}$N nuclear quadrupolar coupling constant of pristine $α\unicode{x2013}$N$_2$ to be $-5.36(2)$ MHz, a significant improvement in accuracy over the previously-accepted value of $-5.39(5)$ MHz, and a validation of our unified description of light-particle ZPM.

cond-mat.str-el↗

arXiv2023

Band-filling-controlled magnetism from transition metal intercalation in $N_{1/3}$NbS$_2$ revealed with first-principles calculations

We present a first-principles study of the effect of 3$d$ transition metal intercalation on the magnetic properties of the 2H-NbS$_2$ system, using spin-resolved density functional theory calculations to investigate the electronic structure of $N_{1/3}$NbS$_2$ ($N$ = Ti, V, Cr, Mn, Fe, Co, Ni). We are able to accurately determine the magnetic moments and crystal field splitting, and find that the magnetic properties of the materials are determined by a mechanism based on filling rigid bands with electrons from the intercalant. We predict the dominant magnetic interaction of these materials by considering Fermi surface nesting, finding agreement with experiment where data are available.

cond-mat.mtrl-sci↗

arXiv2023

High Resolution 3D Strain and Orientation Mapping within a Grain of a Directed Energy Deposition Laser Additively Manufactured Superalloy

The industrialization of Laser Additive Manufacturing (LAM) is challenged by the undesirable microstructures and high residual stresses originating from the fast and complex solidification process. Non-destructive assessment of the mechanical performance controlling deformation patterning is therefore critical. Here, we use Dark Field X-ray Microscopy (DFXM) to non-destructively map the 3D intragranular orientation and strain variations throughout a surface breaking grain within a directed energy deposition nickel superalloy. DFXM results reveal a highly heterogenous 3D microstructure in terms of the local orientation and lattice strain. The grain comprises $\approx$ 5$μ$m-sized cells with alternating strain states, as high as 5 $\times 10^{-3}$, and orientation differences <0.5° . The DFXM results are compared to Electron Backscatter Diffraction measurements of the same grain from its cut-off surface. We discuss the microstructure developments during LAM, rationalising the development of the deformation patterning from the extreme thermal gradients during processing and the susceptibility for solute segregation.

cond-mat.mtrl-sci↗

arXiv2023

First-principles calculations of magnetic states in pyrochlores using a source-corrected exchange and correlation functional

We present a first-principles investigation of the spin-ice state in Dy$_2$Ti$_2$O$_7$ using a magnetic source-free exchange and correlation functional, implemented in the Castep electronic-structure code. By comparing results from the conventional local spin-density approximation, we show that a spin-ice state in Dy$_2$Ti$_2$O$_7$ can be reliably obtained by removing the magnetic sources from the exchange and correlation contributions to the potential, and we contrast this against the computed ground states of other frustrated pyrochlore magnets.

cond-mat.mtrl-sci↗

arXiv2022

Energy-gap driven low-temperature magnetic and transport properties in Cr$_{1/3}M$S$_2$ ($M$ = Nb or Ta)

The helimagnets Cr$_{1/3}M$S$_2$ ($M$ = Nb or Ta) have attracted renewed attention due to the discovery of a chiral soliton lattice (CSL) stabilized in an applied magnetic field, but reports of unusual low-temperature transport and magnetic properties in this system lack a unifying explanation. Here we present electronic structure calculations that demonstrate the materials are half-metals. There is also a gap-like feature (width in range 40-100 meV) in the density of states of one spin channel. This electronic structure explains the low-temperature electronic and magnetic properties of Cr$_{1/3}M$S$_2$ ($M$ = Nb or Ta), with the gap-like feature particularly important for explaining the magnetic behavior. Our magnetometry measurements confirm the existence of this gap. Dynamic spin fluctuations driven by excitations across this gap are seen over a wide range of frequencies (0.1 Hz to MHz) with AC susceptibility and muon-spin relaxation ($μ^+$SR) measurements. We show further how effects due to the CSL in Cr$_{1/3}$NbS$_2$, as detected with $μ^+$SR, dominate over the gap-driven magnetism when the CSL is stabilized as the majority phase.

cond-mat.str-el↗

arXiv2021

Intrinsic nature of spontaneous magnetic fields in superconductors with time-reversal symmetry breaking

We present a systematic investigation of muon-stopping states in superconductors that reportedly exhibit spontaneous magnetic fields below their transition temperatures due to time-reversal symmetry breaking. These materials include elemental rhenium, several intermetallic systems and Sr$_2$RuO$_4$. We demonstrate that the presence of the muon leads to only a limited and relatively localized perturbation to the local crystal structure, while any small changes to the electronic structure occur several electron volts below the Fermi energy leading to only minimal changes in the charge density on ions close to the muon. Our results imply that the muon-induced perturbation alone is unlikely to lead to the observed spontaneous fields in these materials, whose origin is more likely intrinsic to the time-reversal symmetry broken superconducting state.

cond-mat.supr-con↗

arXiv2021

MuFinder: A program to determine and analyse muon stopping sites

Significant progress has recently been made in calculating muon stopping sites using density functional theory. The technique aims to address two of the most common criticisms of the muon-spin spectroscopy ($μ^+$SR) technique, namely, where in the sample does the muon stop, and what is its effect on its local environment. We have designed and developed a program called MuFinder that enables users to carry out these calculations through a simple graphical user interface (GUI). The procedure for calculating muon sites by generating initial muon positions, relaxing the structures, and then clustering and analysing the resulting candidate sites, can be done entirely within the GUI. The local magnetic field at the muon site can also be computed, allowing the connection between the muon sites obtained and experiment to be made. MuFinder will make these computations significantly more accessible to non-experts and help to establish muon site calculations as a routine part of $μ^+$SR experiments.

cond-mat.str-el↗

arXiv2021

Anomalous magnetic exchange in a dimerized quantum-magnet composed of unlike spin species

We present here a study of the magnetic properties of the antiferromagnetic dimer material CuVOF$_4$(H$_2$O)$_6\cdot$H$_2$O, in which the dimer unit is composed of two different $S = 1/2$ species, Cu(II) and V(IV). An applied magnetic field of $μ_0H_{\rm c1} = 13.1(1)~\rm T$ is found to close the singlet-triplet energy gap, the magnitude of which is governed by the antiferromagnetic intradimer, $J_0 \approx 21~\rm K$, and interdimer, $J' \approx 1~\rm K$, exchange energies, determined from magnetometry and electron-spin resonance measurements. The results of density functional theory (DFT) calculations are consistent with the experimental results and predicts antiferromagnetic coupling along all nearest-neighbor bonds, with the magnetic ground state comprising spins of different species aligning antiparallel to one another, while spins of the same species are aligned parallel. The magnetism in this system cannot be accurately described by the overlap between localized V orbitals and magnetic Cu orbitals lying in the Jahn-Teller (JT) plane, with a tight-binding model based on such a set of orbitals incorrectly predicting that interdimer exchange should be dominant. DFT calculations indicate significant spin density on the bridging oxide, suggesting instead an unusual mechanism in which intradimer exchange is mediated through the O atom on the Cu(II) JT axis.

cond-mat.str-el↗

arXiv2020

Megahertz dynamics in skyrmion systems probed with muon-spin relaxation

We present longitudinal-field muon-spin relaxation (LF $μ$SR) measurements on two systems that stabilize a skyrmion lattice (SkL): Cu$_2$OSeO$_3$, and Co$_x$Zn$_y$Mn$_{20-x-y}$ for $(x,y)~=~(10,10)$, $(8,9)$ and $(8,8)$. We find that the SkL phase of Cu$_2$OSeO$_3$ exhibits emergent dynamic behavior at megahertz frequencies, likely due to collective excitations, allowing the SkL to be identified from the $μ$SR response. From measurements following different cooling protocols and calculations of the muon stopping site, we suggest that the metastable SkL is not the majority phase throughout the bulk of this material at the fields and temperatures where it is often observed. The dynamics of bulk Co$_8$Zn$_9$Mn$_3$ are well described by $\simeq~2$ GHz excitations that reduce in frequency near the critical temperature, while in Co$_8$Zn$_8$Mn$_4$ we observe similar behavior over a wide range of temperatures, implying that dynamics of this kind persist beyond the SkL phase.

cond-mat.str-el↗

arXiv2020

Origin of Magnetic Ordering in a Structurally-Perfect Quantum Kagome Antiferromagnet

The ground state of the simple Heisenberg nearest-neighbor quantum kagome antiferromagnetic model is a magnetically disordered spin liquid, yet various perturbations may lead to fundamentally different states. Here we disclose the origin of magnetic ordering in the structurally-perfect kagome material YCu$_3$(OH)$_6$Cl$_3$, which is free of the widespread impurity problem. {\it Ab-initio} calculations and modeling of its magnetic susceptibility reveal that, similar to the archetypal case of herbertsmithite, the nearest-neighbor exchange is by far the dominant isotropic interaction. Dzyaloshinskii-Moriya (DM) magnetic anisotropy deduced from electron spin resonance and specific-heat measurements is, however, significantly larger than in herbertsmithite. By enhancing spin correlations within kagome planes, this anisotropy is essential for magnetic ordering. Our study isolates the effect of DM anisotropy from other perturbations and unambiguously confirms the theoretical phase diagram.

cond-mat.str-el↗

arXiv2020

Magnetism and Néel skyrmion dynamics in GaV$_{4}$S$_{8-y}$Se$_{y}$

We present an investigation of the influence of low-levels of chemical substitution on the magnetic ground state and N{\' e}el skyrmion lattice (SkL) state in GaV$_4$S$_{8-y}$Se$_y$, where $y =0, 0.1, 7.9$, and $8$. Muon-spin spectroscopy ($μ$SR) measurements on $y=0$ and 0.1 materials reveal the magnetic ground state consists of microscopically coexisting incommensurate cycloidal and ferromagnetic environments, while chemical substitution leads to the growth of localized regions of increased spin density. $μ$SR measurements of emergent low-frequency skyrmion dynamics show that the SkL exists under low-levels of substitution at both ends of the series. Skyrmionic excitations persist to temperatures below the equilibrium SkL in substituted samples, suggesting the presence of skyrmion precursors over a wide range of temperatures.

cond-mat.str-el↗

arXiv2019

Local magnetism, magnetic order and spin freezing in the 'nonmetallic metal' FeCrAs

We present the results of x-ray scattering and muon-spin relaxation ($μ^{+}$SR) measurements on the iron-pnictide compound FeCrAs. Polarized non-resonant magnetic x-ray scattering results reveal the 120$^\circ$ periodicity expected from the suggested three-fold symmetric, non-collinear antiferromagnetic structure. $μ^+$SR measurements indicate a magnetically ordered phase throughout the bulk of the material below $T_\mathrm{N}$=105(5) K. There are signs of fluctuating magnetism in a narrow range of temperatures above $T_\mathrm{N}$ involving low-energy excitations, while at temperatures well below $T_\mathrm{N}$ behaviour characteristic of freezing of dynamics is observed, likely reflecting the effect of disorder in our polycrystalline sample. Using density functional theory we propose a distinct muon stopping site in this compound and assess the degree of distortion induced by the implanted muon.

cond-mat.str-el↗