arXiv subjects

A. T. Boothroyd

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

At least 55 records · Page 3Linked to original sources

arXiv2014

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ~ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state.

cond-mat.mtrl-sci↗

arXiv2014

An anisotropic local modification of crystal field levels in Pr-based pyrochlores: a muon-induced effect modelled using density functional theory

Muon spin relaxation measurements on some quantum spin ice candidate materials, the insulating pyrochlores Pr2B2O7 (B = Sn, Zr, Hf), have been performed for temperatures in the range 0.05-280 K. The results are indicative of a static distribution of magnetic moments which appears to grow on cooling and whose size at low temperatures is significantly larger than that expected for Pr nuclear moments. Using density functional theory we show how this effect can be explained via a hyperfine enhancement arising from a splitting of the non-Kramers doublet ground states on Pr ions close to the muon which itself causes a highly anisotropic distortion field. We provide a quantitative relationship between this effect and the measured temperature dependence of the muon relaxation and discuss the relevance of these observations to muon experiments in other frustrated magnetic materials.

cond-mat.str-el↗

arXiv2014

Coupling of magnetic order to planar Bi electrons in the anisotropic Dirac metals AMnBi2 (A = Sr, Ca)

We report powder and single crystal neutron diffraction measurements of the magnetic order in AMnBi2 (A = Sr and Ca), two layered manganese pnictides with anisotropic Dirac fermions on a Bi square net. Both materials are found to order at TN approx 300 K in k = 0 antiferromagnetic structures, with ordered Mn moments at T = 10 K of approximately 3.8 muB aligned along the c axis. The magnetic structures are Neel-type within the Mn--Bi layers but the inter-layer ordering is different, being antiferromagnetic in SrMnBi2 and ferromagnetic in CaMnBi2. This allows a mean-field coupling of the magnetic order to Bi electrons in CaMnBi2 but not in SrMnBi2. We find clear evidence that magnetic order influences electrical transport. First principles calculations explain the experimental observations and suggest that the mechanism for different inter-layer ordering in the two compounds is the competition between the anteiferromagnetic superexchange and ferromagnetic double exchange carried by itinerant Bi electrons.

cond-mat.str-el↗

arXiv2014

Magnetic excitation spectrum of LuFe2O4 measured with inelastic neutron scattering

We report neutron inelastic scattering measurements and analysis of the spectrum of magnons propagating within the Fe2O4 bilayers of LuFe2O4. The observed spectrum is consistent with six magnetic modes and a single prominent gap, which is compatible with a single bilayer magnetic unit cell containing six spins. We model the magnon dispersion by linear spin-wave theory and find very good agreement with the domain-averaged spectrum of a spin-charge bilayer superstructure comprising one Fe3+ -rich monolayer and one Fe2+ -rich monolayer. These findings indicate the existence of polar bilayers in LuFe2O4, contrary to recent studies that advocate a charge-segregated non-polar bilayer model. Weak scattering observed below the magnon gap suggests that a fraction of the bilayers contain other combinations of charged monolayers not included in the model. Refined values for the dominant exchange interactions are reported.

cond-mat.str-el↗

arXiv2014

Crystal field splitting in Sr$_{n+1}$Ir$_n$O$_{3n+1}$ ($n$ = 1, 2) iridates probed by x-ray Raman spectroscopy

Non-resonant Raman spectroscopy in the hard X-ray regime has been used to explore the electronic structure of the first two members of the Ruddlesden-Popper series Sr$_{n+1}$Ir$_n$O$_{3n+1}$ of iridates. By tuning the photon energy transfer around 530 eV we have been able to explore the oxygen K near edge structure with bulk sensitivity. The angular dependence of the spectra has been exploited to assign features in the 528-535 eV energy range to specific transitions involving the Ir 5d orbitals. This has allowed us to extract reliable values for both the t2g-eg splitting arising from the cubic component of the crystal field (10Dq), in addition to the splitting of the eg orbitals due to tetragonal distortions. The values we obtain are (3.8, 1.6) eV and (3.55, 1.9) eV for Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, respectively.

cond-mat.str-el↗

arXiv2014

Stripe disorder and dynamics in the hole-doped antiferromagnetic insulator La5/3Sr1/3CoO4

We report on an investigation into the dynamics of the stripe phase of La5/3Sr1/3CoO4, a material recently shown to have an hour-glass magnetic excitation spectrum. A combination of magnetic susceptibility, muon-spin relaxation and nuclear magnetic resonance measurements strongly suggest that the physics is determined by a disordered configuration of charge and spin stripes whose frustrated magnetic degrees of freedom are strongly dynamic at high temperature and which freeze out in a glassy manner as the temperature is lowered. Our results broadly confirm a recent theoretical prediction, but show that the charge quenching remains incomplete well below the charge ordering temperature and reveal, in detail, the manner in which the magnetic degrees of freedom are frozen.

cond-mat.str-el↗

arXiv2014

Circularly Polarised X-ray Scattering Investigation of Spin-Lattice Coupling in TbMnO$_3$ in Crossed Electric and Magnetic Fields

We present a study of the magnetic and crystallographic structure of TbMnO$_3$ in the presence of crossed electric and magnetic fields using circularly polarised X-ray non-resonant scattering. A comprehensive account is presented of the scattering theory and data analysis methods used in our earlier studies, and in addition we present new high magnetic field data and its analysis. We discuss in detail how polarisation analysis was used to reveal structural information, including the arrangement of Tb moments which we proposed for $H = 0$ T, and how the diffraction data for $H H_C$ as for $H < H_C$. Finally some observations regarding the kinetics and the conservation of domain population at the transition are described.

cond-mat.str-el↗

arXiv2013

Crystal field states in a Quantum Spin Ice]{Crystal field states of Pr$^{3+}$ in the candidate quantum spin ice Pr$_{2}$Sn$_{2}$O$_{7}$

Neutron time-of-flight spectroscopy has been employed to study the crystal-field splitting of Pr$^{3+}$ in the pyrochlore stannate Pr$_{2}$Sn$_{2}$O$_{7}$. The crystal field has been parameterized from a profile fit to the observed neutron spectrum. The single-ion ground state is a well isolated non-Kramers doublet of $Γ_3^+$ symmetry with a large Ising-like anisotropy, $χ_{zz} /χ_\perp \approx 60$ at 10 K, but with a significant admixture of terms $| M_J \neq \pm J >$ which can give rise to quantum zero-point fluctuations. This magnetic state satisfies the requirements for quantum spin ice behavior.

cond-mat.str-el↗

arXiv2013

Absence of strong magnetic fluctuations in the iron phosphide superconductors LaFePO and Sr2ScO3FeP

We report neutron inelastic scattering measurements on polycrystalline LaFePO and Sr2ScO3FeP, two members of the iron phosphide families of superconductors. No evidence is found for any magnetic fluctuations in the spectrum of either material in the energy and wavevector ranges probed. Special attention is paid to the wavevector at which spin-density-wave-like fluctuations are seen in other iron-based superconductors. We estimate that the magnetic signal, if present, is at least a factor of four (Sr2ScO3FeP) or seven (LaFePO) smaller than in the related iron arsenide and chalcogenide superconductors. These results suggest that magnetic fluctuations are not as influential on the electronic properties of the iron phosphide systems as they are in other iron-based superconductors.

cond-mat.supr-con↗

arXiv2013

The Hour-Glass Magnetic Spectrum Arising from a Striped, Cluster Spin Glass Ground State in La1.75Sr0.25CoO4

We report inelastic neutron scattering results that reveal an hour-glass magnetic excitation spectrum in La1.75Sr0.25CoO4. The magnetic spectrum is similar to that observed previously in La1.67Sr0.33CoO4, but the spectral features are broader. We show that the spectrum of La1.75Sr0.25CoO4 can be modeled by the spin dynamics of a system with a disordered cluster spin glass ground state. Bulk magnetization measurements are presented which support the proposed glassy ground state. The observations reiterate the importance of quasi-one-dimensional magnetic correlations and disorder for the hour-glass spectrum, and suggest that disordered spin and charge stripes exist at lower doping in La2-xSrxCoO4 than previously thought.

cond-mat.str-el↗

arXiv2013

Spin fluctuations away from (pi,0) in the superconducting phase of molecular-intercalated FeSe

Magnetic fluctuations in the molecular-intercalated FeSe superconductor Li{x}(ND2){y}(ND3){1-y}Fe2Se2 (Tc = 43K) have been measured by inelastic neutron scattering from a powder sample. The strongest magnetic scattering is observed at a wave vector Q ~ 1.4 A^{-1}, which is not consistent with the (pi,0) nesting wave vector that characterizes magnetic fluctuations in several other iron-based superconductors, but is close to the (pi, pi/2) position found for A{x}Fe{2-y}Se2 systems. At the energies probed (~ 5kB Tc), the magnetic scattering increases in intensity with decreasing temperature below Tc, consistent with the superconductivity-induced magnetic resonance found in other iron-based superconductors.

cond-mat.supr-con↗

arXiv2012

Ground state in a half-doped manganite distinguished by neutron spectroscopy

We have measured the spin-wave spectrum of the half-doped bilayer manganite Pr(Ca,Sr)2Mn2O7 in its spin, charge, and orbital ordered phase. The measurements, which extend throughout the Brillouin zone and cover the entire one-magnon spectrum, are compared critically with spin-wave calculations for different models of the electronic ground state. The data are described very well by the Goodenough model, which has weakly interacting ferromagnetic zig-zag chains in the CE-type arrangement. A model that allows ferromagnetic dimers to form within the zigzags is inconsistent with the data. The analysis conclusively rules out the strongly bound dimer (Zener polaron) model.

cond-mat.str-el↗

arXiv2012

Strongly momentum-dependent screening dynamics in La$_{0.5}$Sr$_{1.5}$MnO$_4$ observed with resonant inelastic x-ray scattering

We report strongly momentum-dependent local charge screening dynamics in CE-type charge, orbital, and spin ordered La$_{0.5}$Sr$_{1.5}$MnO$_4$, based on Mn K-edge resonant inelastic x-ray scattering data. Through a comparison with theoretical calculations, we show that the observed momentum dependence reflects highly localized, nearest neighbor screening of the transient local charge perturbation in this compound with an exciton-like screening cloud, rather than delocalized screening. The size of the screening cloud is estmated to be about 0.4-0.5 interatomic distances.

cond-mat.str-el↗

arXiv2012

The J_{eff}=1/2 insulator Sr3Ir2O7 studied by means of angle-resolved photoemission spectroscopy

The low-energy electronic structure of the J_{eff}=1/2 spin-orbit insulator Sr3Ir2O7 has been studied by means of angle-resolved photoemission spectroscopy. A comparison of the results for bilayer Sr3Ir2O7 with available literature data for the related single-layer compound Sr2IrO4 reveals qualitative similarities and similar J_{eff}=1/2 bandwidths for the two materials, but also pronounced differences in the distribution of the spectral weight. In particuar, photoemission from the J_{eff}=1/2 states appears to be suppressed. Yet, it is found that the Sr3Ir2O7 data are in overall better agreement with band-structure calculations than the data for Sr2IrO4.

cond-mat.str-el↗

arXiv2012

Spin-wave excitations and superconducting resonant mode in Cs(x)Fe(2-y)Se2

We report neutron inelastic scattering measurements on the normal and superconducting states of single-crystalline Cs0.8Fe1.9Se2. Consistent with previous measurements on Rb(x)Fe(2-y)Se2, we observe two distinct spin excitation signals: (i) spin-wave excitations characteristic of the block antiferromagnetic order found in insulating A(x)Fe(2-y)Se2 compounds, and (ii) a resonance-like magnetic peak localized in energy at 11 meV and at an in-plane wave vector of (0.25, 0.5). The resonance peak increases below Tc = 27 K, and has a similar absolute intensity to the resonance peaks observed in other Fe-based superconductors. The existence of a magnetic resonance in the spectrum of Rb(x)Fe(2-y)Se2 and now of Cs(x)Fe(2-y)Se2 suggests that this is a common feature of superconductivity in this family. The low energy spin-wave excitations in Cs0.8Fe1.9Se2 show no measurable response to superconductivity, consistent with the notion of spatially separate magnetic and superconducting phases.

cond-mat.supr-con↗

arXiv2012

An x-ray diffraction study of the temperature-induced structural phase transitions in SmVO3

Through powder x-ray diffraction we have investigated the structural behavior of SmVO3, in which orbital and magnetic degrees of freedom are believed to be closely coupled to the crystal lattice. We have found, contrary to previous reports, that SmVO3 exists in a single, monoclinic, phase below 200 K. The associated crystallographic distortion is then stabilized through the magnetostriction that occurs below 134 K. The crystal structure has been refined using synchrotron x-ray powder diffraction data measured throughout the structural phase diagram, showing a substantial Jahn-Teller distortion of the VO6 octahedra in the monoclinic phase, compatible with the expected G-type orbital order. Changes in the vanadium ion crystal field due to the structural and magnetic transitions have then been probed by resonant x-ray diffraction.

cond-mat.str-el↗

arXiv2012

Microstructural analysis of phase separation in iron chalcogenide superconductors

The interplay between superconductivity, magnetism and crystal structure in iron-based superconductors is a topic of great interest amongst the condensed matter physics community as it is thought to be the key to understanding the mechanisms responsible for high temperature superconductivity. Alkali metal doped iron chalcogenide superconductors exhibit several unique characteristics which are not found in other iron-based superconducting materials such as antiferromagnetic ordering at room temperature, the presence of ordered iron vacancies and high resistivity normal state properties. Detailed microstructural analysis is essential in order to understand the origin of these unusual properties. Here we have used a range of complementary scanning electron microscope based techniques, including high-resolution electron backscatter di raction mapping, to assess local variations in composition and lattice parameter with high precision and sub-micron spatial resolution. Phase separation is observed in the Csx Fe2-ySe2 crystals, with the minor phase distributed in a plate-like morphology throughout the crystal. Our results are consistent with superconductivity occurring only in the minority phase.

cond-mat.supr-con↗

arXiv2012

The Magnetic Structure of DyMn2O5 Determined by Resonant X-ray Scattering

Resonant magnetic x-ray scattering has been used to investigate the magnetic structure of the magnetoelectric multiferroic DyMn2O5. We have studied the magnetic structure in the ferroelectric phase of this material, which displays the strongest ferroelectric polarisation and magnetodielectric effect of the RMn2O5 (where R is a rare earth ion, Y or Bi) family. The magnetic structure observed is similar to that of the other members of the series, but differs in the direction of the ordered moments. In DyMn2O5 both the Dy and Mn moments lie close to the b-axis, whereas in other RMn2O5 they lie close to the a-axis.

cond-mat.str-el↗