arXiv subjects

P. A. Goddard

Publications and source records attributed to P. A. Goddard.

At least 19 recordsLinked to original sources

arXiv2026

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.

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arXiv2025

Single-ion anisotropy driven chiral magnetic order in a spin-1 antiferromagnetic chain

Chirality in magnetic systems gives rise to a wide range of exotic phenomena, yet its influence in $S=1$ chains remains largely unexplored. Here, we present a comprehensive experimental study of a chiral antiferromagnetic (AFM) $S=1$ chain, [Ni(pym)(H$_{2}$O)$_{4}$]SO$_{4} \cdot$ H$_{2}$O (pym = pyrimidine), where the Ni(II) octahedral orientation exhibits a four-fold chiral periodicity. Muon spin rotation measurements indicate the onset of long-range magnetic order below $T_{\rm N} = 1.82(2)\,\mathrm{K}$. Neutron diffraction measurements reveal a chiral AFM order driven by a chiral modulation of the easy-axis anisotropy direction, rather than the typical scenario of Dzyaloshinskii-Moriya interactions, geometrical frustration or higher-order interactions. Inelastic neutron scattering (INS) measurements reveal dispersive spin-wave excitations well described by linear spin-wave theory, with Hamiltonian parameters $J_{0} = 6.81(1)\,\mathrm{K}$ (intrachain exchange), $J'_{1\rm a} = -0.091(1)\,\mathrm{K}$ (interchain exchange), and $D = -3.02(1)\,\mathrm{K}$ (easy-axis single-ion anisotropy). These parameters are further validated by Monte Carlo simulations of the magnetisation. Additionally, the INS data reveal multiple dispersionless bands, suggesting the presence of further excitations beyond the scope of our linear spin-wave theory.

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arXiv2024

Pseudo-easy-axis anisotropy in antiferromagnetic $S=1$ diamond-lattice systems Ni$X_{2}$(pym)$_{2}$

We investigate the magnetic properties of $S=1$ antiferromagnetic diamond lattice, Ni$X_{2}$(pyrimidine)$_{2}$ ($X$ = Cl, Br), hosting a single-ion anisotropy (SIA) orientation which alternates between neighbouring sites. Through neutron diffraction measurements of the $X$ = Cl compound, the ordered state spins are found to align collinearly along a pseudo-easy-axis, a unique direction created by the intersection of two easy planes. Similarities in the magnetization, exhibiting spin-flop transitions, and the magnetic susceptibility in the two compounds imply that the same magnetic structure and a pseudo-easy-axis is also present for $X$ = Br. We estimate the Hamiltonian parameters by combining analytical calculations and Monte-Carlo (MC) simulations of the spin-flop and saturation field. The MC simulations also reveal that the spin-flop transition occurs when the applied field is parallel to the pseudo-easy-axis. Contrary to conventional easy-axis systems, there exist field directions perpendicular to the pseudo-easy-axis for which the magnetic saturation is approached asymptotically and no symmetry-breaking phase transition is observed at finite fields.

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arXiv2024

Magnetic properties of a staggered $S=1$ chain Ni(pym)(H$_{2}$O)$_{2}$(NO$_{3}$)$_{2}$ with an alternating single-ion anisotropy direction

Materials composed of spin-1 antiferromagnetic (AFM) chains are known to adopt complex ground states which are sensitive to the single-ion-anisotropy (SIA) energy ($D$), and intrachain ($J_{0}$) and interchain ($J'_{i}$) exchange energy scales. While theoretical and experimental studies have extended this model to include various other energy scales, the effect of the lack of a common SIA axis is not well explored. Here we investigate the magnetic properties of Ni(pyrimidine)(H$_{2}$O)$_{2}$(NO$_{3}$)$_{2}$, a chain compound where the tilting of Ni octahedra leads to a 2-fold alternation of the easy-axis directions along the chain. Muon-spin relaxation measurements indicate a transition to long-range order at $T_{\text{N}}=2.3$\,K and the magnetic structure is initially determined to be antiferromagnetic and collinear using elastic neutron diffraction experiments. Inelastic neutron scattering measurements were used to find $J_{0} = 5.107(7)$\,K, $D = 2.79(1)$\,K, $J'_{2}=0.18(3)$\,K and a rhombic anisotropy energy $E=0.19(9)$\,K. Mean-field modelling reveals that the ground state structure hosts spin canting of $ϕ\approx6.5^{\circ}$, which is not detectable above the noise floor of the elastic neutron diffraction data. Monte-Carlo simulation of the powder-averaged magnetization, $M(H)$, is then used to confirm these Hamiltonian parameters, while single-crystal $M(H)$ simulations provide insight into features observed in the data.

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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.

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arXiv2024

Magnetotransport of single crystal Sm$_2$Ir$_2$O$_7$ across the pressure-induced quantum-critical phase boundary

Rare-earth pyrochlore iridates host two interlocking magnetic sublattices of corner-sharing tetrahedra and can harbour a unique combination of frustrated moments, exotic excitations and highly correlated electrons. They are also the first systems predicted to display both topological Weyl semimetal and axion insulator phases. We have measured the transport and magnetotransport properties of single-crystal Sm$_2$Ir$_2$O$_7$ up to and beyond the pressure-induced quantum critical point for all-in-all-out (AIAO) Ir order at $p_{\rm c}$ = 63 kbar previously identified by resonant X-ray scattering and close to which Weyl semimetallic behavior has been previously predicted. Our findings overturn the accepted expectation that the suppression of AIAO order should lead to metallic conduction persisting down to zero temperature. Instead, the resistivity-minimum temperature, which tracks the decrease in the AIAO ordering temperature for pressures up to 30~kbar, begins to increase under further application of pressure, pointing to the presence of a second as-yet unidentified mechanism leading to non-metallic behavior. The magnetotransport does track the suppression of Ir magnetism, however, with a strong hysteresis observed only within the AIAO phase boundary, similar to that found for Ho$_2$Ir$_2$O$_7$ and attributed to plastic deformation of Ir domains. Around $p_{\rm c}$ we find the emergence of a new type of electronic phase, characterized by a negative magnetoresistance with small hysteresis at the lowest temperatures, and hysteresis-free positive magnetoresistance above approximately 5 K. The temperature dependence of our low-temperature transport data are found to be best described by a model consistent with a Weyl semimetal across the entire pressure range.

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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.

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arXiv2021

Pressure-induced shift of effective Ce valence, Fermi energy and phase boundaries in CeOs$_4$Sb$_{12}$

CeOs$_4$Sb$_{12}$, a member of the skutterudite family, has an unusual semimetallic low-temperature $\cal{L}$-phase that inhabits a wedge-like area of the field $H$ - temperature $T$ phase diagram. We have conducted measurements of electrical transport and megahertz conductivity on CeOs$_4$Sb$_{12}$ single crystals under pressures of up to 3 GPa and in high magnetic fields of up to 41 T to investigate the influence of pressure on the different $H$-$T$ phase boundaries. While the high-temperature valence transition between the metallic $\cal{H}$-phase and the $\cal{L}$-phase is shifted to higher $T$ by pressures of the order of 1 GPa, we observed only a marginal suppression of the $\cal{S}$-phase that is found below 1 K for pressures of up to 1.91 GPa. High-field quantum oscillations have been observed for pressures up to 3.0 GPa and the Fermi surface of the high-field side of the $\cal{H}$-phase is found to show a surprising decrease in size with increasing pressure, implying a change in electronic structure rather than a mere contraction of lattice parameters. We evaluate the field-dependence of the effective masses for different pressures and also reflect on the sample dependence of some of the properties of CeOs$_4$Sb$_{12}$ which appears to be limited to the low-field region.

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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.

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arXiv2021

Magnetic order and disorder in a quasi-two-dimensional quantum Heisenberg antiferromagnet with randomized exchange

We present an investigation of the effect of randomizing exchange strengths in the $S=1/2$ square lattice quasi-two-dimensional quantum Heisenberg antiferromagnet (QuinH)$_2$Cu(Cl$_{x}$Br$_{1-x}$)$_{4}\cdot$2H$_2$O (QuinH$=$Quinolinium, C$_9$H$_8$N$^+$), with $0\leq x \leq 1$. Pulsed-field magnetization measurements allow us to estimate an effective in-plane exchange strength $J$ in a regime where exchange fosters short-range order, while the temperature $T_{\mathrm{N}}$ at which long range order (LRO) occurs is found using muon-spin relaxation, allowing us to construct a phase diagram for the series. We evaluate the effectiveness of disorder in suppressing $T_{\mathrm{N}}$ and the ordered moment size and find an extended disordered phase in the region $0.4 \lesssim x \lesssim 0.8$ where no magnetic order occurs, driven by quantum effects of the exchange randomness.

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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.

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arXiv2020

Extremely well isolated 2D spin-$1/2$ antiferromagnetic Heisenberg layers with small exchange coupling in the molecular-based magnet CuPOF

We report on a comprehensive characterization of the newly synthesized Cu$^{2+}$-based molecular magnet [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ (CuPOF), where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, $μ^+$SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the 2D square-lattice $S=1/2$ antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of $J/k_\mathrm{B} = 6.80(5)$ K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to $XY$ type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature $XY$ anisotropy under the influence of the interlayer coupling, occurs at $T_\mathrm{N} = 1.38(2)$ K, as revealed by $μ^+$SR. In applied magnetic fields, our $^1$H-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at $T_\mathrm{N} =2.8$ K and 7 T.

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arXiv2020

Magnetic order and ballistic spin transport in a sine-Gordon spin chain

We report the results of muon-spin spectroscopy ($μ^+$SR) measurements on the staggered molecular spin chain [pym-Cu(NO$_3$)$_2$(H$_2$O)$_2$] (pym = pyrimidine), a material previously described using sine-Gordon field theory. Zero-field $μ^+$SR reveals a long range magnetically-ordered ground state below a transition temperature $T_\mathrm{N}=0.22(1)$ K. Using longitudinal-field (LF) $μ^+$SR we investigate the dynamic response in applied magnetic fields $0< B < 500$ mT and find evidence for ballistic spin transport. Our LF $μ^+$SR measurements on the chiral spin chain [Cu(pym)(H$_2$O)$_4$]SiF$_6 \cdot $H$_2$O instead demonstrate one-dimensional spin diffusion and the distinct spin transport in these two systems likely reflects differences in their magnetic excitations.

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arXiv2019

Unusual phase boundary of the magnetic-field-tuned valence transition in CeOs$_4$Sb$_{12}$

The phase diagram of the filled skutterudite CeOs$_4$Sb$_{12}$ has been mapped in fields $H$ of up to 60 T and temperatures $T$ down to 0.5 K using resistivity, magnetostriction, and MHz conductivity. The valence transition separating the semimetallic, low-$H$, low-$T$, $\cal{L}$ phase from the metallic high-$H$, high-$T$ $\cal{H}$ phase exhibits a very unusual, wedge-shaped phase boundary, with a non-monotonic gradient alternating between positive and negative. This is quite different from the text-book "elliptical" phase boundary usually followed by valence transitions. Analysis of Shubnikov-de Haas oscillations within the $\cal{H}$ phase reveals an effective mass that increases as $H$ drops toward the $\cal{H-L}$ phase boundary, suggesting proximity to a quantum-critical point. The associated magnetic fluctuations may be responsible for the anomalous $H,T$ dependence of the valence transition at high $H$, whereas the low$-H$, high$-T$ portion of the phase boundary may rather be associated with the proximity of CeOs$_4$Sb$_{12}$ to a topological semimetal phase induced by uniaxial stress.

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arXiv2019

Unconventional field-induced spin gap in an $S = 1/2$ chiral staggered chain

We investigate the low-temperature magnetic properties of the molecule-based chiral spin chain [Cu(pym)(H$_2$O)$_4$]SiF$_6\cdot$H$_2$O (pym = pyrimidine). Electron-spin resonance, magnetometry and heat capacity measurements reveal the presence of staggered $g$ tensors, a rich low-temperature excitation spectrum, a staggered susceptibility and a spin gap that opens on the application of a magnetic field. These phenomena are reminiscent of those previously observed in non-chiral staggered chains, which are explicable within the sine-Gordon quantum-field theory. In the present case, however, although the sine-Gordon model accounts well for the form of the temperature-dependence of the heat capacity, the size of the gap and its measured linear field dependence do not fit with the sine-Gordon theory as it stands. We propose that the differences arise due to additional terms in the Hamiltonian resulting from the chiral structure of [Cu(pym)(H$_2$O)$_4$]SiF$_6\cdot$H$_2$O, particularly a uniform Dzyaloshinskii-Moriya coupling and a four-fold periodic staggered field.

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arXiv2017

Adiabatic physics of an exchange-coupled spin-dimer system: magnetocaloric effect, zero-point fluctuations, and possible two-dimensional universal behavior

We present the magnetic and thermal properties of the bosonic-superfluid phase in a spin-dimer network using both quasistatic and rapidly-changing pulsed magnetic fields. The entropy derived from a heat-capacity study reveals that the pulsed-field measurements are strongly adiabatic in nature and are responsible for the onset of a significant magnetocaloric effect (MCE). In contrast to previous predictions we show that the MCE is not just confined to the critical regions, but occurs for all fields greater than zero at sufficiently low temperatures. We explain the MCE using a model of the thermal occupation of exchange-coupled dimer spin-states and highlight that failure to take this effect into account inevitably leads to incorrect interpretations of experimental results. In addition, the heat capacity in our material is suggestive of an extraordinary contribution from zero-point fluctuations and appears to indicate universal behavior with different critical exponents at the two field-induced critical points. The data are consistent with a two-dimensional nature of spin excitations in the system.

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arXiv2016

Broken rotational symmetry on the Fermi surface of a high-T$_\mathrm{c}$ superconductor

Broken fourfold rotational (C$_4$) symmetry is observed in the experimental properties of several classes of unconventional superconductors. It has been proposed that this symmetry breaking is important for superconducting pairing in these materials, but in the high superconducting transition temperature (high-T$_{\mathrm{c}}$) cuprates this broken symmetry has never been observed on the Fermi surface. We have measured a pronounced anisotropy in the angle dependence of the interlayer magnetoresistance of the underdoped high-T$_{\mathrm{c}}$) superconductor YBa$_2$Cu$_3$O$_{6.58}$, directly revealing broken C$_4$ symmetry on the Fermi surface. Moreover, we demonstrate that this Fermi surface has C$_2$ symmetry of the type produced by a uniaxial or anisotropic density-wave phase. This establishes the central role of C$_4$ symmetry breaking in the Fermi surface reconstruction of YBa$_2$Cu$_3$O$_{6+δ}$, and suggests a striking degree of universality among unconventional superconductors.

cond-mat.supr-con↗

arXiv2015

Robustness of superconductivity to structural disorder in Sr$_{0.3}$(NH$_2$)$_{y}$(NH$_3$)$_{1-y}$Fe$_2$Se$_2$

The superconducting properties of a recently discovered high $T_{\rm c}$ superconductor, Sr/ammonia-intercalated FeSe, have been measured using pulsed magnetic fields down to $4.\,\rm {K}$ and muon spin spectroscopy down to $1.5\,\rm K$. This compound exhibits intrinsic disorder resulting from random stacking of the FeSe layers along the $c$-axis that is not present in other intercalates of the same family. This arises because the coordination requirements of the intercalated Sr and ammonia moieties imply that the interlayer stacking (along $c$) involves a translation of either ${\bf a}/2$ or ${\bf b}/2$ which locally breaks tetragonal symmetry. The result of this stacking arrangement is that the Fe ions in this compound describe a body-centred tetragonal lattice in contrast to the primitive arrangement of Fe ions described in all other Fe-based superconductors. In pulsed magnetic fields the upper critical field $H_{\text{c2}}$ was found to increase on cooling with an upwards curvature that is commonly seen in type-II superconductors of a multi-band nature. Fitting the data to a two-band model and extrapolation to absolute zero gave a maximum upper critical field ${μ_0H_{\rm c2}(0)}$ of ${33(2)\,\rm T}$. A clear superconducting transition with a diamagnetic shift was also observed in transverse-field muon measurements at ${T_{\text c}\approx36.3(2)\,\rm K}$. These results demonstrate that robust superconductivity in these intercalated FeSe systems does not rely on perfect structural coherence along the $c$-axis.

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