arXiv subjects

Paul A. Goddard

Publications and source records attributed to Paul A. Goddard.

At least 19 recordsLinked to original sources

arXiv2026

Resolving the Magnetic Ground State and Field-Induced Transitions in Magnetic Dirac Semimetal Candidate EuMnSb$_2$

The magnetic structure of a magnetic topological semimetal EuMnSb$_2$ is investigated in fields up to 30 T using polarized and unpolarized neutron diffraction, pulsed-field x-ray magnetic circular dichroism and pulsed-field magnetometry. We determine the zero-field magnetic structures of the Eu and Mn sublattices, and find that magnetic transitions induced by applied fields below 2 T correspond to changes in the magnetic order of the Eu spins alone without detectable perturbation to the order of the Mn spins. An additional magnetic transition is observed at fields close to the saturation field for the Eu spins. We present a mean-field model which describes key features of the magnetic behavior and allows us to estimate the dominant Eu--Eu and Eu--Mn exchange interactions responsible for the coupling between magnetism and electronic topology.

cond-mat.str-el↗

arXiv2026

Gapped 1/9 Magnetization Plateau in the Anisotropic Kagome Antiferromagnet Y-kapellasite

Fractional magnetization plateaus provide a sensitive probe of many-body spin states in frustrated quantum magnets, yet their microscopic origin in kagome antiferromagnets remains unresolved. This is particularly true of the mysterious $1/9$ plateau, which is predicted by theory but infrequently observed in experiment. Here, we investigate this problem in the $S = 1/2$ anisotropic kagome antiferromagnet Y-kapellasite, Y$_3$Cu$_9$(OH)$_{19}$Cl$_8$, using pulsed-field magnetization measurements on single crystals and high-field $^{35}$Cl NMR. We identify a hierarchy of field-induced fractional features, including $1/3$ and $1/9$ plateaus, as well as a weaker low-field feature. Analysis of the NMR spectra and the magnetic susceptibility across the $1/9$ plateau demonstrate that it is accompanied by an ordered local spin configuration, a strong suppression of low-energy spin fluctuations and activated behavior, consistent with a gapped fractional state. These features differ from those in the only other material YCu$_3$(OH)$_6$Br$_2$[Br$_{1-y}$(OH)$_y$] in which this plateau is observed, implying a surprising robustness of the $1/9$ state to the details of the underlying magnetism.

cond-mat.str-el↗

arXiv2025

A resonant valence bond spin liquid in the dilute limit of doped frustrated Mott insulators

Ideas about resonant valence bond liquids and spin-charge separation have led to key concepts in physics such as quantum spin liquids, emergent gauge symmetries, topological order, and fractionalisation. Despite extensive efforts to demonstrate the existence of a resonant valence bond phase in the Hubbard model that originally motivated the concept, a definitive realisation has yet to be achieved. Here we present a solution to this long-standing problem by uncovering a resonant valence bond phase exhibiting spin-charge separation in realistic Hamiltonians. We show analytically that this ground state emerges in the dilute-doping limit of a half-filled Mott insulator on corner-sharing tetrahedral lattices with frustrated hopping, in the absence of exchange interactions. We confirm numerically that the results extend to finite exchange interactions, finite-sized systems and finite dopant density. Although much attention has been devoted to the emergence of unconventional states from geometrically frustrated interactions, our work demonstrates that kinetic energy frustration in doped Mott insulators may be essential for stabilising robust, topologically ordered states in real materials.

cond-mat.str-el↗

arXiv2025

Fermi surface and effective masses of IrO$_2$ probed by de Haas-van Alphen quantum oscillations

Iridium-containing conducting materials are widely investigated for their strong spin-orbit coupling and potential topological properties. Recently the commonly used electrode material iridium dioxide was found to host a large spin-Hall conductivity and was shown to support Dirac nodal lines. Here we present quantum-oscillation experiments on high-quality IrO$_2$ single crystals using the de Haas-van Alphen effect measured using torque magnetometry with a piezo-resistive microcantilever as well as density functional theory-based band-structure calculations. The angle, temperature and field dependencies of the oscillations and the calculated band dispersion provide valuable information on the properties of the charge carriers, including the Fermi-surface geometry and electronic correlations. Comparison of experimental results to calculations allows us to assigns the observed de Haas-van Alphen frequencies to the calculated Fermi surface topology. We find that the effective masses of IrO$_2$ are enhanced compared to the rest electron mass $m_e$, ranging from 1.9 to 3.0~$m_e$, whereas the scattering times indicate excellent sample quality. We discuss our results in context with recent ARPES and band-structure calculation results that found Dirac nodal lines in IrO$_2$ and compare the effective masses and other electronic properties to those of similar materials like the nodal chain metal ReO$_2$ in which Dirac electrons with very light effective masses have been observed.

cond-mat.str-el↗

arXiv2025

Magnetic-field-induced ordering in a spin-1/2 chiral chain

We present neutron diffraction, muon spin rotation and pulsed-field magnetometry measurements on the Heisenberg quantum chiral chain [Cu(pym)(H2O)4]SiF6.H2O, which displays a four-fold-periodic rotation of the local environment around the Cu(II) S = 1/2 ions from site to site along the chain. Previous measurements on this material have shown the absence of magnetic order down to surprisingly low temperatures >= 20 mK, as well as the presence of an energy gap for magnetic excitations that grows linearly with magnetic field. Here we find evidence at dilution refrigerator temperatures for a field-induced transition to long-range magnetic order above an applied magnetic field of 3 T. From the polarization of magnetic moments observed in applied fields we can identify the static magnetic structure that best accounts for the data. The proposed model is supported microscopically by the presence of an alternating component of the g tensor, which produces an internal two-fold staggered field that dictates both the direction of the ordered moments and the effective coupling between adjacent chains. The observed magnetic structure is contrary to previous proposals for the departure of the magnitude and field dependence of the energy gap from the predictions of the sine-Gordon model.

cond-mat.str-el↗

arXiv2025

Spin dynamics in the Dirac $U(1)$ spin liquid YbZn$_2$GaO$_5$

YbZn$_2$GaO$_5$ is a promising candidate for realizing a quantum spin liquid (QSL) state, particularly owing to its lack of significant site disorder. Pulsed-field magnetometry at 0.5 K shows magnetization saturating near 15 T, with a corrected saturation moment of 2.1(1) $μ_\mathrm{B}$ after subtracting the van Vleck contribution. Our zero-field $μ$SR measurements down to milliKelvin temperatures provide evidence for a dynamic ground state and the absence of magnetic order. To probe fluctuations in the local magnetic field at the muon site, we performed longitudinal field $μ$SR experiments. These results provide evidence for spin dynamics with a field dependence that is consistent with a U1A01 Dirac QSL as a plausible description of the ground state.

cond-mat.str-el↗

arXiv2023

Direct evidence from high-field magnetotransport for a dramatic change of quasiparticle character in van der Waals ferromagnet Fe$_{3-x}$GeTe$_2$

Magnetometry and magnetoresistance (MR) data taken on the van der Waals ferromagnet Fe$_{3-x}$GeTe$_2$ (FGT) reveal three distinct contributions to the MR: a linear negative component, a contribution from closed Fermi-surface orbits, and a $H^2$ enhancement linked to a non-coplanar spin arrangement. Contrary to earlier studies on FGT, by accounting for the field dependence of the anomalous Hall effect, we find that the ordinary Hall coefficient decreases markedly below 80 K, indicating a significant change in character of the electrons and holes on the Fermi surface at this temperature. The resulting altered ground state eventually causes the Hall coefficient to reverse sign at 35 K. Our Hall data support the proposal that Kondo-lattice behavior develops in this $d$-electron material below 80 K. Additional evidence comes from the negative linear component of the MR, which arises from electron-magnon scattering with an atypical temperature dependence attributable to the onset of Kondo screening.

cond-mat.str-el↗

arXiv2021

Magnetic ground-state of the one-dimensional ferromagnetic chain compounds $M$(NCS)$_2$(thiourea)$_2$; $M$ = Ni, Co

The magnetic properties of the two isostructural molecule-based magnets, Ni(NCS)$_{2}$(thiourea)$_{2}$, $S$ = 1, [thiourea = SC(NH$_2$)$_2$] and Co(NCS)$_{2}$(thiourea)$_{2}$, $S$ = 3/2, are characterised using several techniques in order to rationalise their relationship with structural parameters and ascertain magnetic changes caused by substitution of the spin. Zero-field heat capacity and muon-spin relaxation measurements reveal low-temperature long-range ordering in both compounds, in addition to Ising-like ($D < 0$) single-ion anisotropy ($D_{\rm{Co}} \sim$ -100 K, $D_{\rm{Ni}} \sim$ -10 K). Crystal and electronic structure, combined with DC-field magnetometry, affirm highly quasi-one-dimensional behaviour, with ferromagnetic intrachain exchange interactions $J_{\rm{Co}}\approx+4$ K and $J_{\rm{Ni}}\sim+100$ K and weak antiferromagnetic interchain exchange, on the order of $J'$ $\sim-0.1$ K. Electron charge and spin-density mapping reveals through-space exchange as a mechanism to explain the large discrepancy in $J$-values despite, from a structural perspective, the highly similar exchange pathways in both materials. Both species can be compared to the similar compounds $M$Cl$_2$(thiourea)$_4$, $M$ = Ni(II) (DTN) and Co(II) (DTC), where DTN is know to harbour two magnetic field-induced quantum critical points. Direct comparison of DTN and DTC with the compounds studied here shows that substituting the halide Cl$^-$ ion, for the NCS$^-$ ion, results in a dramatic change in both the structural and magnetic properties.

cond-mat.str-el↗

arXiv2020

SquidLab -- a user-friendly program for background subtraction and fitting of magnetization data

We present an open-source program free to download for academic use with full user-friendly graphical interface for performing flexible and robust background subtraction and dipole fitting on magnetization data. For magnetic samples with small moment sizes or sample environments with large or asymmetric magnetic backgrounds, it can become necessary to separate background and sample contributions to each measured raw voltage measurement before fitting the dipole signal to extract magnetic moments. Originally designed for use with pressure cells on a Quantum Design MPMS3 SQUID magnetometer, SquidLab is a modular object-oriented platform implemented in Matlab with a range of importers for different widely-available magnetometer systems (including MPMS, MPMS-XL, MPMS-IQuantum, MPMS3 and S700X models), and has been tested with a broad variety of background and signal types. The software allows background subtraction of baseline signals, signal preprocessing, and performing fits to dipole data using Levenberg-Marquadt non-linear least squares, or a singular value decomposition linear algebra algorithm which excels at picking out noisy or weak dipole signals. A plugin system allows users to easily extend the built-in functionality with their own importers, processes or fitting algorithms. SquidLab can be downloaded, under Academic License, from the University of Warwick depository (wrap.warwick.ac.uk/129665).

physics.data-an↗

arXiv2019

A Near-Ideal Molecule-Based Haldane Spin-Chain

The molecular coordination complex NiI$_2$(3,5-lut)$_4$ [where (3,5-lut) $=$ (3,5-lutidine) $=$ (C$_7$H$_9$N)] has been synthesized and characterized by several techniques including synchrotron X-ray diffraction, ESR, SQUID magnetometry, pulsed-field magnetization, inelastic neutron scattering and muon spin relaxation. Templated by the configuration of 3,5-lut ligands the molecules pack in-registry with the Ni--I$\cdots$I--Ni chains aligned along the $c$--axis. This arrangement leads to through-space I$\cdots$I magnetic coupling which is directly measured for the first time in this work. The net result is a near-ideal realization of the $S = 1$ Haldane chain with $J = 17.5~\rm{K}$ and energy gaps of $Δ^{\parallel} = 5.3~{\rm K}$ $Δ^{\perp} =7.7~{\rm K}$, split by the easy-axis single-ion anisotropy $D=-1.2~{\rm K}$. The ratio $D/J = -0.07$ affords one of the most isotropic Haldane systems yet discovered, while the ratio $Δ_0/J = 0.40(1)$ (where $Δ_0$ is the average gap size) is close to its ideal theoretical value, suggesting a very high degree of magnetic isolation of the spin chains in this material. The Haldane gap is closed by orientation-dependent critical fields $μ_0H_{\rm c}^{\parallel} = 5.3~\rm{T}$ and $μ_0H_{\rm c}^{\perp} = 4.3~\rm{T}$, which are readily accessible experimentally and permit investigations across the entirety of the Haldane phase, with the fully polarized state occurring at $μ_0 H_{\rm s}^{\parallel}=46.0~\rm{T}$ and $μ_0 H_{\rm s}^{\perp}=50.7~\rm{T}$. The results are explicable within the so-called fermion model, in contrast to other reported easy-axis Haldane systems. Zero-field magnetic order is absent down to $20~{\rm mK}$ and emergent end-chain effects are observed in the gapped state, as evidenced by detailed low-temperature measurements.

cond-mat.str-el↗

arXiv2019

Determining the anisotropy and exchange parameters of polycrystalline spin-1 magnets

Although low-dimensional $S = 1$ antiferromagnets remain of great interest, difficulty in obtaining high-quality single crystals of the newest materials hinders experimental research in this area. Polycrystalline samples are more readily produced, but there are inherent problems in extracting the magnetic properties of anisotropic systems from powder data. Following a discussion of the effect of powder-averaging on various measurement techniques, we present a methodology to overcome this issue using thermodynamic measurements. In particular we focus on whether it is possible to characterise the magnetic properties of polycrystalline, anisotropic samples using readily available laboratory equipment. We test the efficacy of our method using the magnets [Ni(H$_{2}$O)$_{2}$(3,5-lutidine)$_{4}$](BF$_{4}$)$_{2}$ and Ni(H$_{2}$O)$_{2}$(acetate)$_{2}$(4-picoline)$_{2}$, which have negligible exchange interactions, as well as the antiferromagnet [Ni(H$_{2}$O)$_{2}$(pyrazine)$_{2}$](BF$_{4}$)$_{2}$, and show that we are able to extract the anisotropy parameters in each case. The results obtained from the thermodynamic measurements are checked against electron-spin resonance and neutron diffraction. We also present a density functional method, which incorporates spin-orbit coupling to estimate the size of the anisotropy in [Ni(H$_{2}$O)$_{2}$(pyrazine)$_{2}$](BF$_{4}$)$_{2}$.

cond-mat.str-el↗

arXiv2018

Field-induced canting of magnetic moments in GdCo5 at finite temperature: first-principles calculations and high-field measurements

We present calculations and experimental measurements of the temperature-dependent magnetization of a single crystal of GdCo$_5$ in magnetic fields of order 60 T. At zero temperature the calculations, based on density-functional theory in the disordered-local-moment picture, predict a field-induced transition from an antiferromagnetic to a canted alignment of Gd and Co moments at 46.1 T. At higher temperatures the calculations find this critical field to increase along with the zero-field magnetization. The experimental measurements observe this transition to occur between 44-48 T at 1.4 K. Up to temperatures of at least 100 K, the experiments continue to observe the transition; however, at variance with the calculations, no strong temperature dependence of the critical field is apparent. We assign this difference to the inaccurate description of the zero-field magnetization of the calculations at low temperatures, due to the use of classical statistical mechanics. Correcting for this effect, we recover a consistent description of the high-field magnetization of GdCo$_5$ from theory and experiment.

cond-mat.mtrl-sci↗

arXiv2016

Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a $S = 1$ quantum antiferromagnet

The magnetic ground state of the quasi-one-dimensional spin-1 antiferromagnetic chain is sensitive to the relative sizes of the single-ion anisotropy ($D$) and the intrachain ($J$) and interchain ($J'$) exchange interactions. The ratios $D/J$ and $J'/J$ dictate the material's placement in one or other of three competing phases: a Haldane gapped phase, a quantum paramagnet and an XY-ordered state, with a quantum critical point at their junction. We have identified [Ni(HF)$_2$(pyz)$_2]$SbF$_6$, where pyz = pyrazine, as a candidate in which this behavior can be explored in detail. Combining neutron scattering (elastic and inelastic) in applied magnetic fields of up to 10~tesla and magnetization measurements in fields of up to 60~tesla with numerical modeling of experimental observables, we are able to obtain accurate values of all of the parameters of the Hamiltonian [$D = 13.3(1)$~K, $J = 10.4(3)$~K and $J' = 1.4(2)$~K], despite the polycrystalline nature of the sample. Density-functional theory calculations result in similar couplings ($J = 9.2$~K, $J' = 1.8$~K) and predict that the majority of the total spin population of resides on the Ni(II) ion, while the remaining spin density is delocalized over both ligand types. The general procedures outlined in this paper permit phase boundaries and quantum-critical points to be explored in anisotropic systems for which single crystals are as yet unavailable.

cond-mat.mes-hall↗

arXiv2016

Fermi-surface topologies and low-temperature phases of the filled Skutterudite compounds CeOs$_4$Sb$_{12}$ and NdOs$_4$Sb$_{12}$

MHz conductivity, torque magnetometer and magnetization measurements are reported on single crystals of CeOs$_4$Sb$_{12}$ and NdOs$_4$Sb$_{12}$ using temperatures down to 0.5~K and magnetic fields of up to 60~tesla. The field-orientation dependence of the de Haas-van Alphen and Shubnikov-de Haas oscillations is deduced by rotating the samples about the $[010]$ and $[0\bar{1}1]$ directions. The results indicate that NdOs$_4$Sb$_{12}$ has a similar Fermi surface topology to that of the unusual superconductor PrOs$_4$Sb$_{12}$, but with significantly smaller effective masses, supporting the importance of local phonon modes in contributing to the low-temperature heat capacity of NdOs$_4$Sb$_{12}$. By contrast, CeOs$_4$Sb$_{12}$ undergoes a field-induced transition from an unusual semimetal into a high-field, high-temperature state characterized by a single, almost spherical Fermi-surface section. The behavior of the phase boundary and comparisons with models of the bandstructure lead us to propose that the field-induced phase transition in CeOs$_4$Sb$_{12}$ is similar in origin to the well-known $α-γ$ transition in Ce and its alloys.

cond-mat.str-el↗

arXiv2016

Control of the third dimension in copper-based square-lattice antiferromagnets

Using a mixed-ligand synthetic scheme, we create a family of quasi-two-dimensional antiferromagnets, namely, [Cu(HF$_2$)(pyz)$_2$]ClO$_4$ [pyz = pyrazine], [Cu$L_2$(pyz)$_2$](ClO$_4$)$_2$ [$L$ = pyO = pyridine-N-oxide and 4-phpyO = 4-phenylpyridine-N-oxide. These materials are shown to possess equivalent two-dimensional [Cu(pyz)$_2$]$^{2+}$ nearly square layers, but exhibit interlayer spacings that vary from 6.5713~Å~to 16.777~Å, as dictated by the axial ligands. We present the structural and magnetic properties of this family as determined via x-ray diffraction, electron-spin resonance, pulsed- and quasistatic-field magnetometry and muon-spin rotation, and compare them to those of the prototypical two-dimensional magnetic polymer Cu(pyz)$_2$(ClO$_4$)$_2$. We find that, within the limits of the experimental error, the two-dimensional, {\it intralayer} exchange coupling in our family of materials remains largely unaffected by the axial ligand substitution, while the observed magnetic ordering temperature decreases slowly with increasing layer separation. Despite the structural motifs common to this family and Cu(pyz)$_2$(ClO$_4$)$_2$, the latter has significantly stronger two-dimensional exchange interactions and hence a higher ordering temperature. We discuss these results, as well as the mechanisms that might drive the long-range order in these materials, in terms of departures from the ideal $S=1/2$ two-dimensional square-lattice Heisenberg antiferromagnet. In particular, we find that both spin exchange anisotropy in the intralayer interaction and interlayer couplings (exchange, dipolar, or both) are needed to account for the observed ordering temperatures, with the intralayer anisotropy becoming more important as the layers are pulled further apart.

cond-mat.str-el↗

arXiv2012

Dimensionality selection in a molecule-based magnet

Gaining control of the building blocks of magnetic materials and thereby achieving particular characteristics will make possible the design and growth of bespoke magnetic devices. While progress in the synthesis of molecular materials, and especially coordination polymers, represents a significant step towards this goal, the ability to tune the magnetic interactions within a particular framework remains in its infancy. Here we demonstrate a chemical method which achieves dimensionality selection via preferential inhibition of the magnetic exchange in an $S=1/2$ antiferromagnet along one crystal direction, switching the system from being quasi-two- to quasi-one-dimensional while effectively maintaining the nearest-neighbour coupling strength.

cond-mat.str-el↗

arXiv2011

Low-moment magnetism in the double perovskites Ba2MOsO6 (M=Li,Na)

The magnetic ground states of the isostructural double perovskites Ba$_2$NaOsO$_6$ and Ba$_2$LiOsO$_6$ are investigated with muon-spin rotation. In Ba$_2$NaOsO$_6$ long-range magnetic order is detected via the onset of a spontaneous muon-spin precession signal below $T_{\mathrm{c}}=7.2\pm 0.2\;\mathrm{K}$, while in Ba$_2$LiOsO$_6$ a static but spatially-disordered internal field is found below 8 K. A novel probabilistic argument is used to show from the observed precession frequencies that the magnetic ground state in Ba$_2$NaOsO$_6$ is most likely to be low-moment ($\approx 0.2$\,$μ_{\rm B}$) ferromagnetism and not canted antiferromagnetism. Ba$_2$LiOsO$_6$ is antiferromagnetic and we find a spin-flop transition at 5.5\,T. A reduced osmium moment is common to both compounds, probably arising from a combination of spin-orbit coupling and frustration.

cond-mat.str-el↗

arXiv2008

Magnetic Properties of Ni-Fe Nanowire Arrays: Effect of Template Material and Deposition Conditions

The objective of this work is to study the magnetic properties of arrays of Ni-Fe nanowires electrodeposited in different template materials such as porous silicon, polycarbonate and alumina. Magnetic properties were studied as a function of template material, applied magnetic field (parallel and perpendicular) during deposition, wire length, as well as magnetic field orientation during measurement. The results show that application of magnetic field during deposition strongly influences the c-axis preferred orientation growth of Ni-Fe nanowires. The samples with magnetic field perpendicular to template plane during deposition exhibits strong perpendicular anisotropy with greatly enhanced coercivity and squareness ratio, particularly in Ni-Fe nanowires deposited in polycarbonate templates. In case of polycarbonate template, as magnetic field during deposition increases, both coercivity and squareness ratio also increase. The wire length dependence was also measured for polycarbonate templates. As wire length increases, coercivity and squareness ratio decrease, but saturation field increases. Such magnetic behavior (dependence on template material, magnetic field, wire length) can be qualitatively explained by preferential growth phenomena, dipolar interactio

cond-mat.mtrl-sci↗