arXiv subjects

M. R. Lees

Publications and source records attributed to M. R. Lees.

At least 19 recordsLinked to original sources

arXiv2026

Hidden Magnetic Octupolar Order driven by Spin-Orbit coupling in KFeF$_3$

Phase transitions are typically driven by symmetry-breaking structural distortions that lift electronic degeneracies, yet in some cases, these transitions may be driven by a hidden order without conventional structural signatures. Here, we demonstrate that the 3$d$ perovskite, KFeF$_3$, hosts such a hidden instability. Using a combination of high-resolution powder diffraction, magnetometry, symmetry-based analysis and first principles calculations, we reveal that while the 90 K cubic to rhombohedral transition arises from conventional magnetostriction accompanying antiferromagnetic order, a second transition at 40 K lowers the symmetry to monoclinic without any detectable Jahn-Teller distortion or translational symmetry-breaking. Symmetry-based Landau analysis supports a hidden zone centered magnetic octupole order parameter, whose improper coupling accounts for the weak ferromagnetism and pronounced symmetry-breaking strain. Density functional calculations show that spin-orbit coupling suppresses the competing Jahn-Teller instability, and thereby favors higher rank magnetic multipolar degrees of freedom. These findings establish KFeF$_3$ as a model system in which the competing energy scales between spin-orbit coupling and orbital degeneracy result in the emergence of hidden, multipolar order. We show that the control of such magnetic, multipolar order could, in principle, provide a route to induce altermagnetism.

cond-mat.str-el↗

arXiv2025

A Magnon Band Analysis of GdRu2Si2 in the Field-Polarized State

Understanding the formation of skyrmions in centrosymmetric materials is a problem of fundamental and technological interest. GdRu2Si2 is one such candidate material which has been shown to host a variety of multi-Q magnetic structures, including in zero-field. Here, inelastic neutron scattering is used to measure the spin excitations in the field-polarized phase of GdRu2Si2. Linear spin wave theory and a method of interaction invariant path analysis are used to derive a Hamiltonian accounting for the observed spectra, and comparisons to \textit{ab initio} calculations are made. No evidence for anisotropic or higher order-exchange terms beyond bilinear Heisenberg exchange is found. This is discussed in the context of the multi-Q states existing at lower fields, for which these types of terms have previously been conceived to be significant in the formation of multi-Q ground states.

cond-mat.str-el↗

arXiv2024

Quantum oscillation study of the large magnetoresistance in Mo substituted WTe$_2$ single crystals

The list of interesting electrical properties exhibited by transition metal dichalcogenides has grown with the discovery of extremely large magnetoresistance (MR) and type-II Weyl semimetal behaviour in WTe$_2$ and MoTe$_2$. The extremely large MR in WTe$_2$ is still not adequately understood. Here, we systematically study the effect of Mo substitution on the quantum oscillations in the MR in WTe$_2$. The MR decreases with Mo substitution, however, the carrier concentrations extracted from the quantum oscillations show that the charge compensation improves. We believe that earlier interpretations based on the two-band theory, which attribute the decrease in MR to charge imbalance, could be incorrect due to over-parametrization. We attribute the decrease in MR in the presence of charge compensation to a fall in transport mobility, which is evident from the residual resistivity ratio data. The quantum scattering time and the effective masses do not change within experimental errors upon substitution.

cond-mat.str-el↗

arXiv2024

Ferroelastic control of magnetic domain structure: direct imaging by Magnetic Force Microscopy

Pyrrhotite, Fe$_7$S$_8$, provides an example of exceptionally strong magnetoelastic coupling through pinning of ferromagnetic domains by ferroelastic twins. Using direct imaging of both magnetic and ferroelastic domains by magnetic force microscopy (MFM), the mechanism by which this coupling controls local magnetic switching behaviour of regions on the pyrrhotite surface is revealed, and leads to quantitative fitting of field dependent MFM phase shifts with bulk magnetometry data. It is shown that characteristic inflection points in the magnetometry data along certain direction, in particular $[\overline 120]^*_h$ of the hexagonal parent structure, are in fact caused by ferroelastic pinning of the magnetic moments.

cond-mat.mtrl-sci↗

arXiv2024

Novel quantum spin liquid ground state in the trimer rhodate Ba$_4$NbRh$_3$O$_{12}$

Frustrated magnets offer a plethora of exotic magnetic ground states, including quantum spin liquids (QSLs), in which enhanced quantum fluctuations prevent a long-range magnetic ordering of the strongly correlated spins down to lowest temperature. Here we have investigated the trimer based mixed valence hexagonal rhodate Ba$_4$NbRh$_3$O$_{12}$ using a combination of dc and ac magnetization, electrical resistivity, specific heat, and muon spin rotation/relaxation ($μ$SR) measurements. Despite the substantial antiferromagnetic exchange interactions, as evident from the Weiss temperature ($θ_{\mathrm{W}}\sim -35$ to -45 K), among the Rh-local moments, neither long-range magnetic ordering nor spin-freezing is observed down to at least 50 mK, in ac-susceptibility, specific heat and ZF-$μ$SR measurements (down to 0.26 K). We ascribe the absence of any magnetic transition to enhanced quantum fluctuations as a result of geometrical frustration arising out of the edge-sharing equilateral Rh-triangular network in the structure. Our longitudinal-field $μ$SR result evidences persistent spin fluctuations down to 0.26~K, thus stabilizing a dynamic QSL ground state in Ba$_4$NbRh$_3$O$_{12}$. Furthermore, the magnetic specific heat ($C_{\mathrm{m}}$) data at low-$T$ reveal a significant $T$-linear contribution plus a quadratic $T$-dependence. A $T$-linear behavior is evocative of gapless spin excitations, while the $T^2$-term of $C_{\mathrm{m}}$ may indicate the Dirac QSL phenomenology of the spinon excitations with a linear dispersion.

cond-mat.str-el↗

arXiv2023

The Double-$Q$ Ground State with Topological Charge Stripes in the Skyrmion Candidate $\text{GdRu}_{\text{2}}\text{Si}_{\text{2}}$

$\text{GdRu}_{\text{2}}\text{Si}_{\text{2}}$ is a centrosymmetric magnet in which a skyrmion lattice has recently been discovered. Here, we investigate the magnetic structure of the zero field ground state using neutron diffraction on single crystal and polycrystalline $^{\text{160}}\text{GdRu}_{\text{2}}\text{Si}_{\text{2}}$. In addition to observing the principal propagation vectors $\mathbf{q}_{1}$ and $\mathbf{q}_{2}$, we discover higher order magnetic satellites, notably $\mathbf{q}_{1} + 2\mathbf{q}_{2}$. The appearance of these satellites are explained within the framework of a new double-$Q$ constant-moment solution. Using powder diffraction we implement a quantitative refinement of this model. This structure, which contains vortexlike motifs, is shown to have a one-dimensional topological charge density.

cond-mat.str-el↗

arXiv2022

Nodeless time-reversal symmetry breaking in the centrosymmetric superconductor Sc$_5$Co$_4$Si$_{10}$ probed by muon-spin spectroscopy

We investigate the superconducting properties of Sc$_{5}$Co$_{4}$Si$_{10}$ using low-temperature resistivity, magnetization, heat capacity, and muon-spin rotation and relaxation ($μ$SR) measurements. We find that Sc$_{5}$Co$_{4}$Si$_{10}$ {exhibits type-II} superconductivity with a superconducting transition temperature $T_\mathrm{C}= 3.5 (1)$\,K. The temperature dependence of the superfluid density obtained from transverse-field $μ$SR spectra is best modeled using an isotropic Bardeen-Cooper-Schrieffer type $s$-wave gap symmetry with $2Δ/k_\mathrm{B}T_\mathrm{C} = 2.84(2)$. However, the zero-field muon-spin relaxation asymmetry reveals the appearance of a spontaneous magnetic field below $T_\mathrm{C}$, indicating that time-reversal symmetry (TRS) is broken in the superconducting state. Although this behavior is commonly associated with non-unitary or mixed singlet-triplet pairing, our group-theoretical analysis of the Ginzburg-Landau free energy alongside density functional theory calculations indicates that unconventional mechanisms are pretty unlikely. Therefore, we have hypothesized that TRS breaking may occur via a conventional electron-phonon process.

cond-mat.supr-con↗

arXiv2022

Magnetism in the Néel skyrmion host GaV$_4$S$_8$ under pressure

We present magnetization and muon-spin spectroscopy measurements of Néel skyrmion-host GaV$_4$S$_8$ under the application of hydrostatic pressures up to $P=2.29$ GPa. Our results suggest that the magnetic phase diagram is altered with pressure via a reduction in the crossover temperature from the cycloidal (C) to ferromagnetic-like state with increasing $P$, such that, by 2.29 GPa, the C state appears to persist down to the lowest measured temperatures. With the aid of micromagnetic simulations, we propose that the driving mechanism behind this change is a reduction in the magnetic anisotropy of the system, and suggest that this could lead to an increase in stability of the skyrmion lattice.

cond-mat.str-el↗

arXiv2022

Giant topological and planar Hall effect in Cr$_{1/3}$NbS$_{2}$

Cr$_{1/3}$NbS$_{2}$ is a transition metal dichalcogenide that has been of significant interest due to its ability to host a magnetic chiral soliton lattice. Conventional and planar Hall measurements provide valuable insight into the detection of exotic spin structures in chiral magnets. We show that the presence of a giant planar Hall effect can be attributed to a tilted soliton lattice in Cr$_{1/3}$NbS$_{2}$. Our detailed angular dependent study shows the planar Hall effect and anisotropic magnetoresistance are intrinsically linked in complex non-coplanar magnets. From the conventional Hall signal we show the presence of a giant unconventional, likely topological Hall component, that is the fingerprint of non-coplanar spin textures.

cond-mat.str-el↗

arXiv2022

Effects of Fe deficiency and Co substitution in polycrystalline and single crystals of Fe$_{3}$GeTe$_{2}$

Fe$_{3}$GeTe$_{2}$ is a two-dimensional van der Waals material with a ferromagnetic ground state and a maximum transition temperature $T_{\mathrm{c}}\sim225$ K. However, when Fe$_{3}$GeTe$_{2}$ is synthesized lower values of $T_{\mathrm{c}}$ are often reported. This is attributed to a deficiency in the Fe at the 2c site in the crystal structure. Here we investigate the effect of Fe deficiency and the substitution of Co for Fe on the magnetic properties of this system. We have synthesized both polycrystalline material and single crystals by chemical vapor transport and the flux method, with the largest crystals obtained using the flux method. Cobalt substitution at the Fe site is found to significantly reduce the magnetic transition temperature. Crystals of Fe$_{3}$GeTe$_{2}$ grown by chemical vapor transport with $\sim 8\%$ excess Fe in the starting materials display an optimum Fe content and magnetic transition temperature.

cond-mat.mtrl-sci↗

arXiv2022

Quantum muon diffusion and the preservation of time-reversal symmetry in the superconducting state of type-I rhenium

Elemental rhenium exhibiting type-II superconductivity has been previously reported to break time-reversal symmetry in the superconducting state. We have investigated an arc-melted sample of rhenium exhibiting type-I superconductivity. Low temperature zero-field muon-spin relaxation measurements indicate that time-reversal symmetry is preserved in the superconducting state. Muon diffusion is observed, which is due to quantum mechanical tunneling between interstitial sites. The normal state behavior is characterized by the conduction electrons screening the muons and thermal broadening, and is typical for a metal. Energy asymmetries between muon trapping sites and the superconducting energy gap also characterize the superconducting state behavior.

cond-mat.supr-con↗

arXiv2022

Anisotropic superconductivity and unusually robust electronic critical field in single crystal La$_{7}$Ir$_{3}$

Polycrystalline La$_{7}$Ir$_{3}$ is reported to show superconductivity breaking time-reversal symmetry while also having an isotropic $s$-wave gap. Single crystals of this noncentrosymmetric superconductor are highly desirable to understand the nature of the electron pairing mechanism in this system. Here we report the growth of high-quality single crystals of La$_{7}$Ir$_{3}$ by the Czochralski method. The structural and superconducting properties of these large crystals have been investigated using x-rays, magnetization, resistivity and heat capacity measurements. We observe a clear anisotropy in the lower and upper critical fields for magnetic fields applied parallel and perpendicular to the hexagonal $c$ axis. We also report the presence of a robust electronic critical field, that diverges from the upper critical field derived from heat capacity, which is the hallmark of surface superconductivity.

cond-mat.supr-con↗

arXiv2021

Investigations of the size distribution and magnetic properties of nanoparticles of Cu$_2$OSeO$_3$

Skyrmions in confined geometries have been a subject of increasing interest due to the different properties that they exhibit compared to their bulk counterparts. In this study, nanoparticles of skyrmion-hosting $\text{Cu}_{2}\text{OSeO}_{3}$ have been synthesised using a precipitation method followed by thermal treatment. This enables us to produce nanoparticles whose mean size varies from tens of nanometers to a few micrometers by varying the temperature and duration of the thermal decomposition of the precursor. These sizes span the $\sim 63$~nm diameter of skyrmions in $\text{Cu}_{2}\text{OSeO}_{3}$, allowing investigations into how the magnetic state changes when the size of the geometrical confinement is similar to and smaller than the size of an isolated magnetic skyrmion. AC susceptibility measurements performed on nanoparticles with a size distribution from 15 to 250 nm show a change in the magnetic phase diagram compared to bulk $\text{Cu}_{2}\text{OSeO}_{3}$.

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

Probing the superconducting gap structure in the noncentrosymmetric topological superconductor ZrRuAs

The superconducting gap structure of a topological crystalline insulator (TCI) candidate ZrRuAs ($T^{\rm on}_{\rm c}$ = 7.9(1) K) with a noncentrosymmetric crystal structure has been investigated using muon spin rotation/relaxation ($μ$SR) measurements in transverse-field (TF) and zero-field (ZF) geometries. We also present the results of magnetization, electrical resistivity and heat capacity measurements on ZrRuAs, which reveal bulk superconductivity below 7.9~K. The temperature dependence of the effective penetration depth obtained from the analysis of the TF-$μ$SR spectra below $T_{\rm c}$ is well described by an isotropic $s$-wave gap model as also inferred from an analysis of the heat capacity in the superconducting state. ZF $μ$SR data do not show any significant change in the muon spin relaxation rate above and below the superconducting transition temperature indicating that time-reversal symmetry is preserved in the superconducting state of this material.

cond-mat.supr-con↗

arXiv2021

Investigation of the magnetic ground state of GaV$_4$S$_8$ using powder neutron diffraction

The magnetic ground state of polycrystalline Néel skyrmion hosting material GaV$_4$S$_8$ has been investigated using ac susceptibility and powder neutron diffraction. In the absence of an applied magnetic field GaV$_4$S$_8$ undergoes a transition from a paramagnetic to a cycloidal state below 13~K and then to a ferromagnetic-like state below 6~K. With evidence from ac susceptibility and powder neutron diffraction, we have identified the commensurate magnetic structure at 1.5 K, with ordered magnetic moments of $0.23(2)~μ_{\mathrm{B}}$ on the V1 sites and $0.22(1)~μ_{\mathrm{B}}$ on the V2 sites. These moments have ferromagnetic-like alignment but with a 39(8)$^{\circ}$ canting of the magnetic moments on the V2 sites away from the V$_4$ cluster. In the incommensurate magnetic phase that exists between 6 and 13 K, we provide a thorough and careful analysis of the cycloidal magnetic structure exhibited by this material using powder neutron diffraction.

cond-mat.str-el↗

arXiv2021

Monopole density and antiferromagnetic domain control in spin-ice iridates

Frustration in magnetic systems is fertile ground for complex behaviour, including unconventional ground states with emergent symmetries, topological properties, and exotic excitations. A canonical example is the emergence of magnetic-charge-carrying quasiparticles in spin-ice compounds. Despite extensive work, a reliable experimental indicator of the density of these magnetic monopoles in spin-ice systems is yet to be found. Here, using measurements on single crystals of Ho$_{2}$Ir$_{2}$O$_{7}$ in combination with dipolar Monte Carlo simulations, we show that the magnetoresistance is highly sensitive to the density of monopoles. Moreover, we find that for the orientations of magnetic field in which the monopole density is enhanced, a strong coupling emerges between the magnetic charges on the holmium sublattice and the antiferromagnetically ordered iridium ions, leading to an ability to manipulate the antiferromagnetic domains via a uniform external field. Our results pave the way to a quantitative experimental measure of monopole density and provide a powerful illustration of the interplay between the various magnetic and electronic degrees of freedom in the frustrated pyrochlore iridates. This interdependence holds promise for potential functional properties arising from the link between magnetic and electric charges, as well as for the control of antiferromagnetic domain walls, a key goal in the design of next-generation spintronic devices.

cond-mat.str-el↗

arXiv2021

Chiral singlet superconductivity in the weakly correlated metal LaPt3P

Topological superconductors (SCs) are novel phases of matter with nontrivial bulk topology. They host at their boundaries and vortex cores zero-energy Majorana bound states, potentially useful in fault-tolerant quantum computation. Chiral SCs are particular examples of topological SCs with finite angular momentum Cooper pairs circulating around a unique chiral axis, thus spontaneously breaking time-reversal symmetry (TRS). They are rather scarce and usually feature triplet pairing: best studied examples in bulk materials are UPt3 and Sr2RuO4 proposed to be f-wave and p-wave SCs respectively, although many open questions still remain. Chiral triplet SCs are, however, topologically fragile with the gapless Majorana modes weakly protected against symmetry preserving perturbations in contrast to chiral singlet SCs. Using muon spin relaxation (muSR) measurements, here we report that the weakly correlated pnictide compound LaPt3P has the two key features of a chiral SC: spontaneous magnetic fields inside the superconducting state indicating broken TRS and low temperature linear behaviour in the superfluid density indicating line nodes in the order parameter. Using symmetry analysis, first principles band structure calculation and mean-field theory, we unambiguously establish that the superconducting ground state of LaPt3P is chiral d-wave singlet.

cond-mat.supr-con↗