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P. A. Goddard

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

At least 37 records · Page 2Linked to original sources

The magnetic ground state of two isostructual polymeric quantum magnets, [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ and [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, investigated with neutron powder diffraction

The magnetic ground state of two isostructural coordination polymers (i) the quasi two-dimensional S = 1/2 square-lattice antiferromagnet [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$; and (ii) a new compound [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, were examined with neutron powder diffraction measurements. We find the ordered moments of the Heisenberg S = 1/2 Cu(II) ions in [Cu(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 0.6(1)$μ_{B}$, whilst the ordered moments for the Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ are 3.02(6)$μ_{B}$. For Cu(II), this reduced moment indicates the presence of quantum fluctuations below the ordering temperature. We show from heat capacity and electron spin resonance measurements, that due to the crystal electric field splitting of the S = 3/2 Co(II) ions in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$, this isostructual polymer also behaves as an effective spin-half magnet at low temperatures. The Co moments in [Co(HF$_{2}$)(pyrazine)$_{2}$]SbF$_{6}$ show strong easy-axis anisotropy, neutron diffraction data which do not support the presence of quantum fluctuations in the ground state and heat capacity data which are consistent with 2D or close to 3D spatial exchange anisotropy.

cond-mat.str-el↗

Normal-state nodal electronic structure in underdoped high-Tc copper oxides

An outstanding problem in the field of high-transition-temperature (high Tc) superconductivity is the identification of the normal state out of which superconductivity emerges in the mysterious underdoped regime. The normal state uncomplicated by thermal fluctuations is effectively accessed by the use of applied magnetic fields sufficiently strong to suppress long-range superconductivity at low temperatures. Proposals in which the normal ground state is characterised by small Fermi surface pockets that exist in the absence of symmetry breaking have been superseded by models based on the existence of a superlattice that breaks the translational symmetry of the underlying lattice. Recently, a charge superlattice model that positions a small electron-like Fermi pocket in the vicinity of the nodes (where the superconducting gap is minimum) has been proposed a replacement for the prevalent superlattice models that position the Fermi pocket in the vicinity of the pseudogap at the antinodes (where the superconducting gap is maximum). Although some ingredients of symmetry breaking have been recently revealed by crystallographic studies, their relevance to the electronic structure remains unresolved. Here we report angle-resolved quantum oscillation measurements in the underdoped copper oxide YBa2Cu3O6+x. These measurements reveal a normal ground state comprising electron-like Fermi surface pockets located in the vicinity of the superconducting gap minima (or nodes), and further point to an underlying superlattice structure of low frequency and long wavelength with features in common with the charge order identified recently by complementary spectroscopic techniques.

cond-mat.supr-con↗

Magnetism in a family of $S = 1$ square lattice antiferromagnets Ni$X_2$(pyz)$_2$ ($X = $ Cl, Br, I, NCS; pyz = pyrazine)

The crystal structures of Ni$X_2$(pyz)$_2$ ($X$ = Cl (\textbf{1}), Br (\textbf{2}), I (\textbf{3}) and NCS (\textbf{4})) were determined at 298~K by synchrotron X-ray powder diffraction. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN$_4$$X_2$ units that are bridged by pyz ligands. The 2D layered motifs displayed by \textbf{1}-\textbf{4} are relevant to bifluoride-bridged [Ni(HF$_2$)(pyz)$_2$]$Z$F$_6$ ($Z$ = P, Sb) which also possess the same 2D layers. In contrast, terminal $X$ ligands occupy axial positions in \textbf{1}-\textbf{4} and cause a staggering of adjacent layers. Long-range antiferromagnetic order occurs below 1.5 (Cl), 1.9 (Br and NCS) and 2.5~K (I) as determined by heat capacity and muon-spin relaxation. The single-ion anisotropy and $g$ factor of \textbf{2}, \textbf{3} and \textbf{4} are measured by electron spin resonance where no zero--field splitting was found. The magnetism of \textbf{1}-\textbf{4} crosses a spectrum from quasi-two-dimensional to three-dimensional antiferromagnetism. An excellent agreement was found between the pulsed-field magnetization, magnetic susceptibility and $T_\textrm{N}$ of \textbf{2} and \textbf{4}. Magnetization curves for \textbf{2} and \textbf{4} calculated by quantum Monte Carlo simulation also show excellent agreement with the pulsed-field data. \textbf{3} is characterized as a three-dimensional antiferromagnet with the interlayer interaction ($J_\perp$) slightly stronger than the interaction within the two-dimensional [Ni(pyz)$_2$]$^{2+}$ square planes ($J_\textrm{pyz}$).

cond-mat.str-el↗

The upper critical field of NaFe$_{1-x}$Co$_x$As superconductors

The upper critical field of NaFe$_{1-x}$Co$_x$As was measured from $x=0$ to $x=0.08$, with the magnetic field applied parallel ($H_{\rm c2}^\parallel$) and normal ($H_{\rm c2}^\perp$) to the planes. The data were fitted using one-band and two-band models. The orbital and paramagnetic components of the upper critical field were extracted for $H_{\rm c2}^\parallel$, which we find to to be strongly dominated by paramagnetic pair-breaking. In the parent compound the paramagnetic limit is equal to the value expected by BCS theory. However, substitution of Fe by Co leads to an enhancement above the BCS limit by a factor of approximately 1.6. In the over-doped region, we observe a significant convex curvature in $H_{\rm c2}^\perp$ at low temperatures, which we attribute to the two-band nature of the superconductivity and the asymmetry between the two bands. Additionally, we discuss the behavior of critical field anisotropy, coherence length $ξ$, and the penetration depth $λ$.

cond-mat.supr-con↗

Controlling magnetic order and quantum disorder in one- and zero-dimensional molecule-based magnets

We investigate the structural and magnetic properties of two molecule-based magnets synthesized from the same starting components. Their different structural motifs promote contrasting exchange pathways and consequently lead to markedly different magnetic ground states. Through examination of their structural and magnetic properties we show that [Cu(pyz)(H$_{2}$O)(gly)$_{2}$](ClO$_{4}$)$_{2}$ may be considered a quasi-one-dimensional quantum Heisenberg antiferromagnet while the related compound [Cu(pyz)(gly)](ClO$_{4}$), which is formed from dimers of antiferromagnetically interacting Cu$^{2+}$ spins, remains disordered down to at least 0.03 K in zero field, but shows a field-temperature phase diagram reminiscent of that seen in materials showing a Bose-Einstein condensation of magnons.

cond-mat.str-el↗

Evolution of magnetic interactions in a pressure-induced Jahn-Teller driven magnetic dimensionality switch

We present the results of high-field magnetization and muon-spin relaxation measurements on the coordination polymer CuF_2(H_2O)_2(pyrazine) in pressures up to 22.5 kbar. We observe a transition from a quasi-two-dimensional to a quasi-one-dimensional antiferromagnetic phase at 9.1 kbar, driven by a rotation of the Jahn-Teller axis. Long-range antiferromagnetic ordering is seen in both regimes, as well as a phase separation in the critical pressure region. The magnetic dimensionality switching as pressure is increased is accompanied by a halving of the primary magnetic exchange energy J and a fivefold decrease in the ordering temperature T_N. J decreases gradually with pressure in the two-dimensional phase, and then increases in the one-dimensional regime. We relate both effects to the changes in the crystal structure with applied pressure.

cond-mat.str-el↗

Compensated electron and hole pockets in an underdoped high Tc superconductor

We report quantum oscillations in the underdoped high Tc YBCO over a wide range in magnetic field 28<B<85 T corresponding to ~12 oscillations, enabling the Fermi surface topology to be mapped to high resolution. As earlier reported by Sebastian et al., we find a Fermi surface comprising multiple pockets, as revealed by the additional distinct quantum oscillation frequencies and harmonics reported in this work. We find the originally reported broad low frequency Fourier peak at 535 T to be clearly resolved into three separate peaks at 460 T, 532 T and 602 T. Our increased resolution and angle-resolved measurements identify these frequencies to originate from two similarly sized pockets with greatly contrasting degrees of interlayer corrugation. The spectrally dominant frequency originates from a pocket (α) that is almost ideally two-dimensional in form. In contrast, the newly resolved weaker adjacent spectral features originate from a deeply corrugated pocket (γ). On comparison with band structure, the d-wave symmetry of the interlayer dispersion locates the minimally corrugated αpocket at the 'nodal' point where holes are located in a translational symmetry-broken scenario, and the significantly corrugated γpocket at the 'antinodal' point in the Brillouin zone, where electrons are located in a translational symmetry-broken scenario. Translational symmetry breaking by an SDW is suggested from the strong suppression of Zeeman splitting for the spectrally dominant pocket, additional evidence for which is provided from the harmonics we resolve in the present experiments. Given the similarity in αand γpocket sizes, their opposite carrier type and the previous report of a diverging effective mass, we discuss the possibility of a secondary Fermi surface instability at low dopings of the excitonic insulator type, associated with the metal-insulator QCP.

cond-mat.supr-con↗

A new collective phenomenon arising from spin anisotropic perturbations to a Heisenberg square lattice manifested in paramagnetic resonance experiments

We report unexpected behaviour in a family of Cu spin- 1/2 systems, in which an apparent gap in the low energy magneto-optical absorption spectrum opens at low temperature. This previously unreported collective phenomenon arises at temperatures where the energy of the dominant exchange interaction exceeds the thermal energy. Simulations of the observed shifts in electron paramagnetic resonance spectral weight, which include spin anisotropy, reproduce this behavior yielding the magnitude of the spin anisotropy in these compounds.

cond-mat.str-el↗

Isotope effect in quasi-two-dimensional metal-organic antiferromagnets

Although the isotope effect in superconducting materials is well-documented, changes in the magnetic properties of antiferromagnets due to isotopic substitution are seldom discussed and remain poorly understood. This is perhaps surprising given the possible link between the quasi-two-dimensional (Q2D) antiferromagnetic and superconducting phases of the layered cuprates. Here we report the experimental observation of shifts in the Néel temperature and critical magnetic fields ($ΔT_{\rm N}/T_{\rm N}\approx 4%$; $ΔB_{\rm c}/B_{\rm c}\approx 4%$) in a Q2D organic molecular antiferromagnets on substitution of hydrogen for deuterium. These compounds are characterized by strong hydrogen bonds through which the dominant superexchange is mediated. We evaluate how the in-plane and inter-plane exchange energies evolve as the hydrogens on different ligands are substituted, and suggest a possible mechanism for this effect in terms of the relative exchange efficiency of hydrogen and deuterium bonds.

cond-mat.str-el↗

Exchange parameters of copper-based quasi-two-dimensional Heisenberg magnets measured using high magnetic fields and muon-spin rotation

Pulsed-field magnetization experiments (fields $B$ of up to 85 T and temperatures $T$ down to 0.4 K) are reported on nine organic Cu-based two-dimensional (2D) Heisenberg magnets. All compounds show a low-$T$ magnetization that is concave as a function of $B$, with a sharp ``elbow'' transition to a constant value at a field $B_{\rm c}$. Monte-Carlo simulations including a finite interlayer exchange energy $J_{\perp}$ quantitatively reproduce the data; the concavity indicates the effective dimensionality and $B_{\rm c}$ is an accurate measure of the in-plane exchange energy $J$. Using these values and Neél temperatures measured by muon-spin rotation, it is also possible to obtain a quantitative estimate of $|J_{\perp}/J|$. In the light of these results, it is suggested that in magnets of the form [Cu(HF$_2$)(pyz)$_2$]X, where X is an anion, the sizes of $J$ and $J_{\perp}$ are controlled by the tilting of the pyrazine (pyz) molecule with respect to the 2D planes.

cond-mat.str-el↗

Angle-dependent magnetoresistance oscillations due to magnetic breakdown orbits

We present experimental evidence for a hitherto unconfirmed type of angle-dependent magnetoresistance oscillation caused by magnetic breakdown. The effect was observed in the organic superconductor kappa-(BEDT-TTF)$_2$Cu(NCS)$_2$ using hydrostatic pressures of up to 9.8 kbar and magnetic fields of up to 33 T. In addition, we show that similar oscillations are revealed in ambient pressure measurements, provided that the Shubnikov-de Haas oscillations are suppressed either by elevated temperatures or filtering of the data. These results provide a compelling validation of Pippard's semiclassical picture of magnetic breakdown.

cond-mat.str-el↗

A de Haas-van Alphen study of the filled skutterudite compounds PrOs$_4$As$_{12}$ and LaOs$_4$As$_{12}$

Comprehensive magnetic-field-orientation dependent studies of the susceptibility and de Haas-van Alphen effect have been carried out on single crystals of the filled skutterudites PrOs$_4$As$_{12}$ and LaOs$_4$As$_{12}$ using magnetic fields of up to 40~T. Several peaks are observed in the low-field susceptibility of PrOs$_4$As$_{12}$, corresponding to cascades of metamagnetic transitions separating the low-field antiferromagnetic and high-field paramagnetic metal (PMM) phases. The de Haas-van Alphen experiments show that the Fermi-surface topologies of PrOs$_4$As$_{12}$ in its PMM phase and LaOs$_4$As$_{12}$ are very similar. In addition, they are in reasonable agreement with the predictions of bandstructure calculations for LaOs$_4$As$_{12}$ on the PrOs$_4$As$_{12}$ lattice. Both observations suggest that the Pr 4$f$ electrons contribute little to the number of itinerant quasiparticles in the PMM phase. However, whilst the properties of LaOs$_4$As$_{12}$ suggest a conventional nonmagnetic Fermi liquid, the effects of direct exchange and electron correlations are detected in the PMM phase of PrOs$_4$As$_{12}$. For example, the quasiparticle effective masses in PrOs$_4$As$_{12}$ are found to decrease with increasing field, probably reflecting the gradual suppression of magnetic fluctuations associated with proximity to the low-temperature, low-field antiferromagnetic state.

cond-mat.str-el↗

Separation of energy scales in the kagome antiferromagnet TmAgGe: a magnetic-field-orientation study up to 55 T

TmAgGe is an antiferromagnet in which the spins are confined to distorted kagome-like planes at low temperatures. We report angle-dependent measurements of the magnetization $M$ in fields of up to 55 T that show that there are two distinct and separate energy scales present in TmAgGe, each responsible for a set of step-like metamagnetic transitions; weak exchange interactions and strong crystalline electric field (CEF) interactions. Simulations of $M$ using a three-dimensional, free-energy minimization technique allow us to specify for the first time the physical origin of the metamagnetic transitions in low, in-plane fields. We also show that the transitions observed with the field perpendicular to the kagome planes are associated with the CEF-split multiplet of Tm.

cond-mat.mtrl-sci↗

Role of anisotropy in the spin-dimer compound BaCuSi2O6

We present results of magnetisation and electron paramagnetic resonance experiments on the spin-dimer system BaCuSi2O6. Evidence indicates that the origin of anisotropic terms in the spin Hamiltonian is from magnetic dipolar interactions. Axial symmetry-breaking is on a very small energy scale of ~11 mK, confirming Bose Einstein condensation critical scaling over an extended temperature range in the vicinity of the quantum critical point.

cond-mat.str-el↗

A photonic bandgap resonator to facilitate GHz frequency conductivity experiments in pulsed magnetic fields

We describe instrumentation designed to perform millimeter-wave conductivity measurements in pulsed high magnetic fields at low temperatures. The main component of this system is an entirely non-metallic microwave resonator. The resonator utilizes periodic dielectric arrays (photonic bandgap structures) to confine the radiation, such that the resonant modes have a high Q-factor, and the system possesses sufficient sensitivity to measure small samples within the duration of a magnet pulse. As well as measuring the sample conductivity to probe orbital physics in metallic systems, this technique can detect the sample permittivity and permeability allowing measurement of spin physics in insulating systems. We demonstrate the system performance in pulsed magnetic fields with both electron paramagnetic resonance experiments and conductivity measurements of correlated electron systems.

cond-mat.str-el↗

Recent high-magnetic-field studies of unusual groundstates in quasi-two-dimensional crystalline organic metals and superconductors

After a brief introduction to crystalline organic superconductors and metals, we shall describe two recently-observed exotic phases that occur only in high magnetic fields. The first involves measurements of the non-linear electrical resistance of single crystals of the charge-density-wave (CDW) system (Per)$_2$Au(mnt)$_2$ in static magnetic fields of up to 45 T and temperatures as low as 25 mK. The presence of a fully gapped CDW state with typical CDW electrodynamics at fields higher that the Pauli paramagnetic limit of 34 T suggests the existence of a modulated CDW phase analogous to the Fulde-Ferrell-Larkin-Ovchinnikov state. Secondly, measurements of the Hall potential of single crystals of $α$-(BEDT-TTF)$_2$KHg(SCN)$_4$, made using a variant of the Corbino geometry in quasistatic magnetic fields, show persistent current effects that are similar to those observed in conventional superconductors. The longevity of the currents, large Hall angle, flux quantization and confinement of the reactive component of the Hall potential to the edge of the sample are all consistent with the realization of a new state of matter in CDW systems with significant orbital quantization effects in strong magnetic fields.

cond-mat.supr-con↗

Fermi Surface as a Driver for the Shape-Memory Effect in AuZn

Martensites are materials that undergo diffusionless, solid-state transitions. The martensitic transition yields properties that depend on the history of the material and may allow it to recover its previous shape after plastic deformation. This is known as the shape-memory effect (SME). We have succeeded in identifying the primary electronic mechanism responsible for the martensitic transition in the shape-memory alloy AuZn by using Fermi-surface measurements (de Haas-van Alphen oscillations) and band-structure calculations. This strongly suggests that electronic band structure is an important consideration in the design of future SME alloys.

cond-mat.mtrl-sci↗

Landau quantization effects in the charge-density-wave system (Per)$_2M$(mnt)$_2$ (where $M=$Au and Pt)

A finite transfer integral $t_a$ orthogonal to the conducting chains of a highly one-dimensional metal gives rise to empty and filled bands that simulate an indirect-gap semiconductor upon formation of a commensurate charge-density-wave (CDW). In contrast to semiconductors such as Ge and Si with bandgaps $\sim 1$ eV, the CDW system possesses an indirect gap with a greatly reduced energy scale, enabling moderate laboratory magnetic fields to have a major effect. The consequent variation of the thermodynamic gap with magnetic field due to Zeeman splitting and Landau quantization enables the electronic bandstructure parameters (transfer integrals, Fermi velocity) to be determined accurately. These parameters reveal the orbital quantization limit to be reached at $\sim 20$ T in (Per)$_2M$(mnt)$_2$ salts, making them highly unlikely candidates for a recently-proposed cascade of field-induced charge-density wave states.

cond-mat.str-el↗