arXiv subjects

A. T. Boothroyd

Publications and source records attributed to A. T. Boothroyd.

At least 37 records · Page 2Linked to original sources

arXiv2018

Evidence for $J_{\rm eff} = 0$ ground state and defect-induced spin glass behaviour in the pyrochlore osmate Y$_{2}$Os$_{2}$O$_{7}$

We present AC and DC magnetometry, heat capacity, muon spin relaxation ($μ$SR) and resonant inelastic X-ray scattering (RIXS) studies of the pyrochlore osmate Y$_2$Os$_2$O$_7$. We observe a non-zero effective moment governed by $\sqrt{f}μ_{\rm{eff}} = 0.417(1)\,μ_{\rm{B}}$ where $f$ is the fraction of Os sites which exhibit a spin, and spin freezing at temperature $T_{\rm f} \simeq 5\,$K, consistent with previous results. The field dependence of magnetisation data shows that the paramagnetic moment is most likely due to large moments $μ_{\rm eff} \simeq 3\,μ_{\rm B}$ on only a small fraction $f \simeq 0.02$ of Os sites. Comparison of single-ion energy level calculations with the RIXS data yields a non-magnetic $J_{\rm eff} = 0$ ground state on the Os$^{4+}$ sites. The spin-orbit interaction, Hund's coupling and trigonal distortion of OsO$_{6}$ octahedra are all important in modelling the experimentally observed spectra. We are able to rule out impurity effects, leaving disorder-related effects such as oxygen non-stoichiometry or site interchange between Os and Y ions as the most plausible explanation for the magnetic response in this material.

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arXiv2018

Coupling of magnetic order and charge transport in the candidate Dirac semimetal EuCd$_2$As$_2$

We use resonant elastic x-ray scattering to determine the evolution of magnetic order in EuCd$_2$As$_2$ below $T_\textrm{N}=9.5$\,K, as a function of temperature and applied magnetic field. We find an A-type antiferromagneticstructure with in-plane magnetic moments, and observe dramatic magnetoresistive effects associated with field-induced changes in the magnetic structure and domain populations. Our \textit{ab initio} electronic structure calculations indicate that the Dirac dispersion found in the nonmagnetic Dirac semimetal Cd$_3$As$_2$ is also present in EuCd$_2$As$_2$, but is gapped for $T < T_\textrm{N}$ due to the breaking of $C_3$ symmetry by the magnetic structure.

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arXiv2018

Persistence of antiferromagnetic order upon La substitution in the $4d^4$ Mott insulator Ca$_2$RuO$_4$

The chemical and magnetic structures of the series of compounds Ca$_{2-x}$La$_x$RuO$_4$ [$x = 0$, $0.05(1)$, $0.07(1)$, $0.12(1)$] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low temperature S-Pbca space group of the parent compound is retained in all insulating samples [$x\leq0.07(1)$], but with significant changes to the atomic positions within the unit cell. These changes can be characterised in terms of the local RuO$_6$ octahedral coordination: with increasing doping the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasi-tetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic $k=(0,0,0)$, $b$-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of $x\approx0.11$. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favouring the B mode instead, and to reduce the Néel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the $d^4$ Mott insulator Ca$_2$RuO$_4$, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.

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arXiv2018

Spin dynamics and exchange interactions in CuO measured by neutron scattering

The magnetic properties of CuO encompass several contemporary themes in condensed matter physics, including quantum magnetism, magnetic frustration, magnetically-induced ferroelectricity and orbital currents. Here we report polarized and unpolarized neutron inelastic scattering measurements which provide a comprehensive map of the cooperative spin dynamics in the low temperature antiferromagnetic (AFM) phase of CuO throughout much of the Brillouin zone. At high energies ($E \gtrsim 100$\,meV) the spectrum displays continuum features consistent with the des Cloizeax--Pearson dispersion for an ideal $S=\frac{1}{2}$ Heisenberg AFM chain. At lower energies the spectrum becomes more three-dimensional, and we find that a linear spin-wave model for a Heisenberg AFM provides a very good description of the data, allowing for an accurate determination of the relevant exchange constants in an effective spin Hamiltonian for CuO. In the high temperature helicoidal phase, there are features in the measured low-energy spectrum that we could not reproduce with a spin-only model. We discuss how these might be associated with the magnetically-induced multiferroic behavior observed in this phase.

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arXiv2017

The Final Chapter In The Saga Of YIG

The magnetic insulator Yttrium Iron Garnet can be grown with exceptional quality, has a ferrimagnetic transition temperature of nearly 600 K, and is used in microwave and spintronic devices that can operate at room temperature. The most accurate prior measurements of the magnon spectrum date back nearly 40 years, but cover only 3 of the lowest energy modes out of 20 distinct magnon branches. Here we have used time-of-flight inelastic neutron scattering to measure the full magnon spectrum throughout the Brillouin zone. We find that the existing model of the excitation spectrum, well known from an earlier work titled "The Saga of YIG", fails to describe the optical magnon modes. Using a very general spin Hamiltonian, we show that the magnetic interactions are both longer-ranged and more complex than was previously understood. The results provide the basis for accurate microscopic models of the finite temperature magnetic properties of Yttrium Iron Garnet, necessary for next-generation electronic devices.

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arXiv2017

Doping Dependence of Collective Spin and Orbital Excitations in Spin 1 Quantum Antiferromagnet La$_{2-x}$Sr$_x$NiO$_4$ Observed by X-rays

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to \emph{collective} magnetic excitations in $S=1$ systems by probing the Ni $L_3$-edge of La$_{2-x}$Sr$_x$NiO$_4$ ($x = 0, 0.33, 0.45$). The magnetic excitation peak is asymmetric, indicating the presence of single and multi spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultra-fast pump-probe experiments.

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arXiv2016

Commensurate lattice distortion in the layered titanium oxypnictides Na$_{2}$Ti$_{2}Pn_{2}$O ($Pn =$ As, Sb) determined by X-ray diffraction

We report single crystal X-ray diffraction measurements on Na$_2$Ti$_{2}Pn_{2}$O ($Pn$ = As, Sb) which reveal a charge superstructure that appears below the density wave transitions previously observed in bulk data. From symmetry-constrained structure refinements we establish that the associated distortion mode can be described by two propagation vectors, ${\bf q}_{1} = (1/2, 0, l)$ and ${\bf q}_{2} = (0, 1/2, l)$, with $l=0$ (Sb) or $l = 1/2$ (As), and primarily involves in-plane displacements of the Ti atoms perpendicular to the Ti--O bonds. The results provide direct evidence for phonon-assisted charge density wave order in Na$_2$Ti$_{2}Pn_{2}$O and identify a proximate ordered phase that could compete with superconductivity in doped BaTi$_{2}$Sb$_{2}$O.

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arXiv2016

Spin resonance in the superconducting state of Li$_{1-x}$Fe$_{x}$ODFe$_{1-y}$Se observed by neutron spectroscopy

We have performed inelastic neutron scattering measurements on a powder sample of the superconductor lithium iron selenide hydroxide Li$_{1-x}$Fe$_{x}$ODFe$_{1-y}$Se ($x \simeq 0.16, y \simeq 0.02$, $T_{\rm c} = 41$\,K). The spectrum shows an enhanced intensity below $T_{\rm c}$ over an energy range $0.64\times2Δ< E < 2Δ$, where $Δ$ is the superconducting gap, with maxima at the wave vectors $Q_1 \simeq 1.46$\,Å$^{-1}$ and $Q_2 \simeq 1.97$\,Å$^{-1}$. The behavior of this feature is consistent with the spin resonance mode found in other unconventional superconductors, and strongly resembles the spin resonance observed in the spectrum of the molecular-intercalated iron selenide, Li$_{0.6}$(ND$_{2}$)$_{0.2}$(ND$_{3}$)$_{0.8}$Fe$_{2}$Se$_{2}$. The signal can be described with a characteristic two-dimensional wave vector $(π, 0.67π)$ in the Brillouin zone of the iron square lattice, consistent with the nesting vector between electron Fermi sheets.

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arXiv2016

Inelastic neutron scattering investigations of an anisotropic hybridization gap in the Kondo insulators: CeT2Al10 (T=Fe, Ru and Os)

The recent discovery of topological Kondo insulating behaviour in strongly correlated electron systems has generated considerable interest in Kondo insulators both experimentally and theoretically. The Kondo semiconductors CeT2Al10 (T=Fe, Ru and Os) possessing a c-f hybridization gap have received considerable attention recently because of the unexpected high magnetic ordering temperature of CeRu2Al10 (TN=27 K) and CeOs2Al10 (TN=28.5 K) and the Kondo insulating behaviour observed in the valence fluctuating compound CeFe2Al10 with a paramagnetic ground state down to 50 mK. We are investigating this family of compounds, both in polycrystalline and single crystal form, using inelastic neutron scattering to understand the role of anisotropic c-f hybridization on the spin gap formation as well as on their magnetic properties. We have observed a clear sign of a spin gap in all three compounds from our polycrystalline study as well as the existence of a spin gap above the magnetic ordering temperature in T=Ru and Os. Our inelastic neutron scattering studies on single crystals of CeRu2Al10 and CeOs2Al10 revealed dispersive gapped spin wave excitations below TN. Analysis of the spin wave spectrum reveals the presence of strong anisotropic exchange, along the c-axis (or z-axis) stronger than in the ab-plane. These anisotropic exchange interactions force the magnetic moment to align along the c-axis, competing with the single ion crystal field anisotropy, which prefers moments along the a-axis. In the paramagnetic state (below 50 K) of the Kondo insulator CeFe2Al10, we have also observed dispersive gapped magnetic excitations which transform into quasi-elastic scattering on heating to 100 K. We will discuss the origin of the anisotropic hybridization gap in CeFe2Al10 based on theoretical models of heavy-fermion semiconductors.

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arXiv2016

Direct evidence for charge stripes in a layered cobalt oxide

Recent experiments indicate that static stripe-like charge order is generic to the hole-doped copper oxide superconductors and competes with superconductivity. Here we show that a similar type of charge order is present in La$_{5/3}$Sr$_{1/3}$CoO$_4$, an insulating analogue of the copper oxide superconductors containing cobalt in place of copper. The stripe phase we have detected is accompanied by short-range, quasi-one-dimensional, antiferromagnetic order, and provides a natural explanation for the distinctive hourglass shape of the magnetic spectrum previously observed in neutron scattering measurements of La$_{5/3}$Sr$_{1/3}$CoO$_4$ and many hole-doped copper oxide superconductors. The results establish a solid empirical basis for theories of the hourglass spectrum built on short-range, quasi-static, stripe correlations.

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arXiv2016

All-in all-out magnetic order and propagating spin-waves in Sm2Ir2O7

Using resonant magnetic x-ray scattering we address the unresolved nature of the magnetic groundstate and the low-energy effective Hamiltonian of Sm$_2$Ir$_2$O$_7$, a prototypical pyrochlore iridate with a finite temperature metal-insulator transition. Through a combination of elastic and inelastic measurements, we show that the magnetic ground state is an all-in all-out (AIAO) antiferromagnet. The magnon dispersion indicates significant electronic correlations and can be well-described by a minimal Hamiltonian that includes Heisenberg exchange ($J=27.3(6)$ meV) and Dzyaloshinskii-Moriya interaction ($D=4.9(3)$ meV), which provides a consistent description of the magnetic order and excitations. In establishing that Sm$_2$Ir$_2$O$_7$ has the requisite inversion symmetry preserving AIAO magnetic groundstate, our results support the notion that pyrochlore iridates may host correlated Weyl semimetals.

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arXiv2015

Magnetic phase diagram of La$_{2-x}$Sr$_{x}$CoO$_{4}$ revised using muon-spin relaxation

We report the results of a muon-spin relaxation ($μ$SR) investigation of La$_{2-x}$Sr$_{x}$CoO$_{4}$, an antiferromagnetic insulating series which has been shown to support charge ordered and magnetic stripe phases and an hourglass magnetic excitation spectrum. We present a revised magnetic phase diagram, which shows that the suppression of the magnetic ordering temperature is highly sensitive to small concentrations of holes. Distinct behavior within an intermediate $x$ range ($0.2 \leq x \lesssim 0.6$) suggests that the putative stripe ordered phase extends to lower $x$ than previously thought. Further charge doping ($0.67 \leq x \leq 0.9$) prevents magnetic ordering for $T \gtrsim 1.5~{\rm K}$

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arXiv2015

The importance of XY anisotropy in Sr2IrO4 revealed by magnetic critical scattering experiments

The magnetic critical scattering in Sr$_2$IrO$_4$ has been characterized using X-ray resonant magnetic scattering (XRMS) both below and above the 3D antiferromagnetic ordering temperature, T$_{\text{N}}$. The order parameter critical exponent below T$_{\text{N}}$ is found to be β=0.195(4), in the range of the 2D XYh$_4$ universality class. Over an extended temperature range above T$_{\text{N}}$, the amplitude and correlation length of the intrinsic critical fluctuations are well described by the 2D Heisenberg model with XY anisotropy. This contrasts with an earlier study of the critical scattering over a more limited range of temperature which found agreement with the theory of the isotropic 2D Heisenberg quantum antiferromagnet, developed to describe the critical fluctuations of the conventional Mott insulator La$_2$CuO$_4$ and related systems. Our study therefore establishes the importance of XY anisotropy in the low-energy effective Hamiltonian of Sr$_2$IrO$_4$, the prototypical spin-orbit Mott insulator.

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arXiv2015

Evidence of quantum dimer excitations in Sr$_3$Ir$_2$O$_7$

The magnetic excitation spectrum in the bilayer iridate Sr$_3$Ir$_2$O$_7$ has been investigated using high-resolution resonant inelastic x-ray scattering (RIXS) performed at the iridium L$_3$ edge and theoretical techniques. A study of the systematic dependence of the RIXS spectrum on the orientation of the wavevector transfer, $\mathbf{Q}$, with respect to the iridium-oxide bilayer has revealed that the magnon dispersion is comprised of two branches well separated in energy and gapped across the entire Brillouin zone. Our results contrast with those of an earlier study which reported the existence of a single dominant branch. While these earlier results were interpreted as two overlapping modes within a spin-wave model of weakly coupled iridium-oxide planes, our results are more reminiscent of those expected for a system of weakly coupled dimers. In this latter approach the lower and higher energy modes find a natural explanation as those corresponding to transverse and longitudinal fluctuations, respectively. We have therefore developed a bond-operator theory which describes the magnetic dispersion in Sr$_3$Ir$_2$O$_7$ in terms of quantum dimer excitations. In our model dimerisation is produced by the leading Heisenberg exchange, $J_c$, which couples iridium ions in adjacent planes of the bilayer. The Hamiltonian also includes in plane exchange, $J$, as well as further neighbour couplings and relevant anisotropies. The bond-operator theory provides an excellent account of the dispersion of both modes, while the measured $\mathbf{Q}$ dependence of the RIXS intensities is in reasonable qualitative accord with the spin-spin correlation function calculated from the theory. We discuss our results in the context of the quantum criticality of bilayer dimer systems in the presence of anisotropic interactions derived from strong spin-orbit coupling.

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arXiv2015

Divacancy superstructures in thermoelectric calcium-doped sodium cobaltate

We have grown single crystals of Na$_x$Ca$_y$CoO$_2$ and determined their superstructures as a function of composition using neutron and x-ray diffraction. Inclusion of Ca$^{2+}$ stabilises a single superstructure across a wide range of temperatures and concentrations. The superstructure in the Na$^+$ layers is based on arrays of divacancy clusters with Ca$^{2+}$ ions occupying the central site, and it has an ideal concentration Na$_{4/7}$Ca$_{1/7}$CoO$_2$. Previous measurements of the thermoelectric properties on this system are discussed in light of this superstructure. Na$_{4/7}$Ca$_{1/7}$CoO$_2$ corresponds to the maximum in thermoelectric performance of this system.

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arXiv2015

Two-dimensional Cs-vacancy superstructure in iron-based superconductor $Cs_{0.8}Fe_{1.6}Se_2$

Single crystal neutron diffraction is combined with synchrotron x-ray scattering to identify the different superlattice phases present in $Cs_{0.8}Fe_{1.6}Se_2$. A combination of single crystal refinements and first principles modelling are used to provide structural solutions for the $\sqrt{5}\times\sqrt{5}$ and $\sqrt{2}\times\sqrt{2}$ superlattice phases. The $\sqrt{5}\times\sqrt{5}$ superlattice structure is predominantly composed of ordered Fe vacancies and Fe distortions, whereas the $\sqrt{2}\times\sqrt{2}$ superlattice is composed of ordered Cs vacancies. The Cs vacancies only order within the plane, causing Bragg rods in reciprocal space. By mapping x-ray diffraction measurements with narrow spatial resolution over the surface of the sample, the structural domain pattern was determined, consistent with the notion of a majority antiferromagnetic $\sqrt{5}\times\sqrt{5}$ phase and a superconducting $\sqrt{2}\times\sqrt{2}$ phase.

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arXiv2015

Strong $(π,0)$ spin fluctuations in $β$-FeSe observed by neutron spectroscopy

We have performed powder inelastic neutron scattering measurements on the unconventional superconductor $β$-FeSe ($T_{\rm c} \simeq 8\,\mathrm{K}$). The spectra reveal highly dispersive paramagnetic fluctuations emerging from the square-lattice wave vector $(π,0)$ extending beyond 80 meV in energy. Measurements as a function of temperature at an energy of $\sim 13\,\mathrm{meV}$ did not show any variation from $T_{\rm c}$ to $104\,\mathrm{K}$. The results show that FeSe is close to an instability towards $(π,0)$ antiferromagnetism characteristic of the parent phases of the high-$T_{\rm c}$ iron arsenide superconductors, and that the iron paramagnetic moment is neither affected by the orthorhombic-to-tetragonal structural transition at $T_{\rm s} \simeq 90\,\mathrm{K}$ nor does it undergo a change in spin state over the temperature range studied.

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arXiv2015

Crystal field states of Tb3+ in the pyrochlore spin liquid Tb2Ti2O7 from neutron spectroscopy

We report time-of-flight neutron scattering measurements of the magnetic spectrum of Tb3+ in Tb2Ti2O7. The data, which extend up to 120 meV and have calibrated intensity, enable us to consolidate and extend previous studies of the single-ion crystal field spectrum. We successfully refine a model for the crystal field potential in Tb2Ti2O7 without relying on data from other rare earth titanate pyrochlores, and we confirm that the ground state is a non-Kramers doublet with predominantly |+/-4> components. We compare the model critically with earlier models.

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