arXiv subjects

R. A. Cowley

Publications and source records attributed to R. A. Cowley.

At least 19 recordsLinked to original sources

arXiv2018

Disentangling orbital and spin exchange interactions for Co$^{2+}$ on a rocksalt lattice

Neutron spectroscopy was applied to study the magnetic interactions of orbitally degenerate Co$^{2+}$ on a host MgO rocksalt lattice where no long range spin or orbital order exists. The paramagnetic nature of the substituted monoxide Co$_{0.03}$Mg$_{0.97}$O allows for the disentanglement of spin-exchange and spin-orbit interactions. By considering the prevalent excitations from Co$^{2+}$ spin pairs, we extract 7 exchange constants out to the fourth coordination shell. An antiferromagnetic next nearest neighbor 180$^{\circ}$ exchange interaction is dominant, however dual ferromagnetic and antiferromagnetic interactions are observed for pairings with other pathways. These interactions can be understood in terms of a combination of orbital degeneracy in the $t_{2g}$ channel and the Goodenough-Kanamori-Anderson (GKA) rules. Our work suggests that such a hierarchy of exchange interactions exists in transition metal-based oxides with a $t_{2g}$ orbital degeneracy.

cond-mat.str-el↗

arXiv2014

Phase Transition of the Uniaxial Disordered Ferroelectric Sr$_{0.61}$Ba$_{0.39}$Nb$_2$O$_6$

We report a neutron scattering study of a ferroelectric phase transition in Sr$_{0.61}$Ba$_{0.39}$Nb$_2$O$_6$ (SBN-61). The ferroelectric polarization is along the crystallographic $c$-axis but the transverse acoustic branch propagating along the $<$1, 1, 0$>$ direction does not show any anomaly associated with the this transition. We find no evidence for a soft transverse optic phonon. We do, however, observe elastic diffuse scattering. The intensity of this scattering increases as the sample is cooled from a temperature well above the phase transition. The susceptibility associated with this diffuse scattering follows well the anomaly of the dielectric permittivity of SBN-61. Below T$_\mathrm{c}$ the shape of this scattering is consistent with the scattering expected from ferroelectric domain walls. Our results suggest that despite apparent chemical disorder SBN-61 behaves as a classic order-disorder uniaxial ferroelectric with critical fluctuations in the range $<10^{-11}$ s.

cond-mat.mtrl-sci↗

arXiv2013

Neutron scattering measurements of $dd$ and spin-orbit excitations below the Mott-Hubbard gap in CoO

Neutron scattering is used to investigate the single-ion spin and orbital excitations below the Mott-Hubbard gap in CoO. Three excitations are reported at 0.870 $\pm$ 0.009 eV, 1.84 $\pm$ 0.03, and 2.30 $\pm$ 0.15 eV. These were parameterized within a weak crystal field scheme with an intra-orbital exchange of $J(dd)$=1.3 $\pm$ 0.2 eV and a crystal field splitting 10Dq=0.94 $\pm$ 0.10 eV. A reduced spin-orbit coupling of λ=-0.016 $\pm$ 0.003 eV is derived from dilute samples of Mg$_{0.97}$Co$_{0.03}$O, measured to remove complications due to spin exchange and structural distortion parameters which split the cubic phase degeneracy of the orbital excitations complicating the inelastic spectrum. The 1.84 eV, while reported using resonant x-ray and optical techniques, was absent or weak for non resonant x-ray experiments and overlaps with the expected position of a $^{4}A_{2}$ level. This transition is absent in the dipolar approximation but expected to have a finite quadrupolar matrix element that can be observed with neutron scattering techniques at larger momentum transfers. Our results agree with a crystal field analysis (in terms of Racah parameters and Tanabe-Sugano diagrams) and with previous calculations performed using local-density band theory for Mott insulating transition metal oxides. The results also demonstrate the use of neutron scattering for measuring dipole forbidden transitions in transition metal oxide systems.

cond-mat.str-el↗

arXiv2012

The Structure and Low-Energy Phonons of the Nonferroelectric Mixed Perovskite: BaMg1/3Ta2/3O3

The structure of BaMg1/3Ta2/3O3 (BMT) has been studied using X-ray scattering. The phonons have been measured and the results are similar to those of other materials with the perovskite structure such as PbMg1/3Nb2/3O3 (PMN). The acoustic and lowest energy optic branches were measured but it was not possible to measure the branches of higher energy, possibly this is because they largely consist of oxygen motions. High-resolution inelastic measurements also showed that the diffuse scattering was strictly elastic and not directly related to the phonon spectra. A diffuse scattering was observed in BMT near the (H\pm1/2, K\pm1/2, L\pm1/2) points in the Brillouin zone and this had a characteristic cube shape. This arises from ordering of the B-site ions in BMT. Additional experiments revealed a diffuse scattering in BMT similar in shape to Bragg reflections at wave-vectors of the form (H\pm1/3, K\pm1/3, L\pm1/3). Such reflections were also observed by Lufaso [Chem. Matt. 16 (2004) 2148] from powders and suggest that this structure of BMT consists of 4 differently oriented domains of a trigonal structure and results from a different ordering of the B-site ions from that responsible for the scattering at the (H\pm1/2, K\pm1/2, L\pm1/2) points. The results lead us to suggest that for BMT single crystals the bulk has the properties of a cubic perovskite, whereas the surface may have quite different structure from that of the bulk. This difference resembles the behaviour of cubic relaxors like PMN and PMN doped by PbTiO3, where significant surface effects have been reported.

cond-mat.mtrl-sci↗

arXiv2012

Cube-shape diffuse scattering and the ground state of $\mathrm{BaMg}_{1/3}\mathrm{Ta}_{2/3} \mathrm{O}_3$

A quite unusual diffuse scattering phenomenology was observed in the single-crystal X-ray diffraction pattern of cubic perovskite BMT ($\mathrm{BaMg}_{1/3}\mathrm{Ta}_{2/3}\mathrm{O}_3$). The intensity of the scattering is parametrized as a set of cube-like objects located at the centers of reciprocal space unit cells, resembling very broad and cubic-shaped (1/2,1/2,1/2)-satellites. BMT belongs to perovskites of formula AB$'_{1/3}$B$"_{2/3}$O$_{3}$ (A=Mg, B$'=$Ta, B$"=$Mg). The cubes of the intensity can be attributed to the partial correlations of the occupancies of the B site. The pair correlation function is the Fourier transform of the diffuse scattering intensity and the latter's idealized form yields the unusual property of a power-law correlation decay with distance. Up to now this is observed only in a few exotic instances of magnetic order or nematic crystals. Therefore it cannot be classified as a short-range order phenomenon, as in most situations originating diffuse scattering. A Monte-Carlo search in configuration space yielded solutions that reproduce faithfully the observed diffuse scattering. Analysis of the results in terms of the electrostatic energy and the entropy point to this phase of BMT as a metastable state, kinetically locked, which could be the equilibrium state just below the melting point.

cond-mat.mtrl-sci↗

arXiv2011

Reply to comment by Mayers et al. on "High energy neutron scattering from hydrogen using a direct geometry spectrometer"

In this reply, we point out several criticisms of the analysis in arXiv:0909.2633 and show that the comment does not change the underlying conclusion presented by ourselves that there is no measurable deficit in the scattering cross section of hydrogen. We therefore consider that our original conclusions are correct namely that the previous anomalies in the cross section are due to experimental effects related to the use of indirect geometry spectrometers.

cond-mat.mtrl-sci↗

arXiv2010

The effect of the pseudogap on suppressing high energy inelastic neutron scattering in superconducting YBa2Cu3O6.5

We have measured the spin fluctuations in the YBa2Cu3O6.5 (YBCO6.5, Tc=59 K) superconductor at high-energy transfers above ~ 100 meV. Within experimental error, the momentum dependence is isotropic at high-energies, similar to that measured in the insulator for two dimensional spin waves, and the dispersion extrapolates back to the incommensurate wave vector at the elastic position. This result contrasts with previous expectations based on measurements around 50 meV which were suggestive of a softening of the spin-wave velocity with increased hole doping. Unlike the insulator, we observe a significant reduction in the intensity of the spin excitations for energy transfers above ~ 100 meV similar to that observed above ~ 200 meV in the YBCO6.35 (Tc=18 K) superconductor as the spin waves approach the zone boundary. We attribute this high energy scale with a second gap and find agreement with measurements of the pseudogap in the cuprates associated with electronic anomalies along the antinodal positions. In addition, we observe a sharp peak at around 400 meV whose energy softens with increased hole doping. We discuss possible origins of this excitation including a hydrogen related molecular excitation and a transition of electronic states between d levels.

cond-mat.supr-con↗

arXiv2010

Magnetic excitations of spin and orbital moments in cobalt oxide

Magnetic and phonon excitations in the antiferromagnet CoO with an unquenched orbital angular momentum are studied by neutron scattering. Results of energy scans in several Brillouin zones in the (HHL) plane for energy transfers up to 16 THz are presented. The measurements were performed in the antiferromagnetic ordered state at 6 K (well below TN~290 K) as well as in the paramagnetic state at 450 K. Several magnetic excitation modes are identified from the dependence of their intensity on wavevector and temperature. Within a Hund's rule model the excitations correspond to fluctuations of coupled orbital and spin degrees of freedom whose bandwidth is controlled by interionic superexchange. The different <111> ordering domains give rise to several magnetic peaks at each wavevector transfer.

cond-mat.str-el↗

arXiv2009

Diffuse scattering from the lead-based relaxor ferroelectric PbMg_1/3Ta_2/3O_3

The relaxor ferroelectric PbMg_1/3Ta_2/3O_3 was studied by single-crystal neutron and synchrotron x-ray diffraction and its detailed atomic structure has been modeled in terms of static Pb-displacements that lead to the formation of polar nanoregions. Similar to the other members of the Pb-based relaxor family like PbMg_1/3Nb_2/3O_3 or PbZn_1/3Nb_2/3O_3 the diffuse scattering in the [H,0,0]/[0,K,0] scattering plane has a butterfly-shape around the (h,0,0) Bragg reflections and is transverse to the scattering vector for (h,h,0) peaks. In the [H,H,0]/[0,0,L] plane the diffuse scattering is elongated along the <1,1,2> directions and is transverse to the scattering vector for (h,h,h) reflections. We find that a model consisting of correlated Pb-displacements along the <1,1,1>-directions reproduces the main features of the diffuse scattering in PbMg_1/3Ta_2/3O_3 adequately when the correlation lengths between the Pb-ion displacement vectors are longest along the <1,1,1> and <1,-1,0> and shortest along <1,1,-2> directions.

cond-mat.mtrl-sci↗

arXiv2009

High energy neutron scattering from hydrogen using a direct geometry spectrometer

Deep inelastic neutron scattering experiments using indirect time-of-flight spectrometers have reported a smaller cross section for the hydrogen atom than expected from conventional scattering theory. Typically, at large momentum transfers, a deficit of 20-40% in the neutron scattering intensity has been measured and several theories have been developed to explain these results. We present a different approach to this problem by investigating the hydrogen cross section in polyethylene using the direct geometry time-of-flight spectrometer MARI with the incident energy fixed at a series of values ranging from Ei=0.5 eV to 100 eV. These measurements span a much broader range in momentum than previous studies and with varying energy resolutions. We observe no momentum dependence to the cross section with an error of 4% and through a comparison with the scattering from metal foil standards measure the absolute bound cross section of the hydrogen atom to be sigma(H)= 80 +/- 4 barns. These results are in agreement with conventional scattering theory but contrast with theories invoking quantum entanglement and neutron experiments supporting them. Our results also illustrate a unique use of direct geometry chopper instruments at high incident energies and demonstrate their capability for conducting high-energy spectroscopy.

cond-mat.stat-mech↗

arXiv2008

Soft Modes and Relaxor Ferroelectrics

Relaxor ferroelectrics are difficult to study and understand. The experiment shows that at low energy scattering there is an acoustic mode, an optic mode, dynamic quasi-elastic scattering and strictly elastic scattering as well as Bragg peaks at the zone centre. We have studied the scattering using the TASP spectrometer at PSI and have analysed the data using a model with interactions between the different components particularly to determine the properties of the elastic scattering. The quasi-elastic scattering begins to become significant at the Burns temperature of 620 K. It steadily increases in intensity on cooling reaching a maximum at ~400 K. Below this temperature the strictly elastic scattering begins to increase and shows a broadened line shape characteristic of crystals in a random applied field. We show that all the results obtained from PMN for the elastic scattering are consistent with the crystal having a random field transition at ~400 K. We have obtained similar results for PMN-PT and PZN-PT suggesting that random fields of the nano-regions also play an important role in these materials.

cond-mat.mtrl-sci↗

arXiv2008

A study of the quantum classical crossover in the spin dynamics of the 2D S=5/2 antiferromagnet Rb2MnF4: neutron scattering, computer simulations, and analytic theories

We report comprehensive inelastic neutron scattering measurements of the magnetic excitations in the 2D spin-5/2 Heisenberg antiferromagnet Rb2MnF4 as a function of temperature from deep in the Neel ordered phase up to paramagnetic, 0.13 < kBT/4JS < 1.4. Well defined spin-waves are found for wave-vectors larger than the inverse correlation length $η^{-1}$ for temperatures up to near the Curie-Weiss temperature, $Θ_{CW}$. For wave-vectors smaller than $η^{-1}$, relaxational dynamics occurs. The observed renormalization of spin-wave energies, and evolution of excitation line-shapes, with increasing temperature are quantitatively compared with finite-temperature spin-wave theory, and computer simulations for classical spins. Random phase approximation calculations provide a good description of the low-temperature renormalisation of spin-waves. In contrast, lifetime broadening calculated using the first Born approximation shows, at best, modest agreement around the zone boundary at low temperatures. Classical dynamics simulations using an appropriate quantum-classical correspondence were found to provide a good description of the intermediate- and high-temperature regimes over all wave-vector and energy scales, and the crossover from quantum to classical dynamics observed around $Θ_{CW}/S$, where the spin S=5/2. A characterisation of the data over the whole wave-vector/energy/temperature parameter space is given. In this, $T^2$ behaviour is found to dominate the wave-vector and temperature dependence of the line widths over a large parameter range, and no evidence of hydrodynamic behaviour or dynamical scaling behaviour found within the accuracy of the data sets.

cond-mat.stat-mech↗

arXiv2007

Orbital and Spin Excitations in Cobalt Oxide

By means of neutron scattering we have determined new branches of magnetic excitations in orbitally active CoO (TN=290 K) up to 15 THz and for temperatures from 6 K to 450 K. Data were taken in the (111) direction in six single-crystal zones. From the dependence on temperature and Q we have identified several branches of magnetic excitation. We describe a model for the coupled orbital and spin states of Co2+ subject to a crystal field and tetragonal distortion.

cond-mat.str-el↗

arXiv2007

Evidence for decay of spin-waves above the pseudogap in underdoped YBa2Cu3O6.35

The magnetic spectrum at high-energies in heavily underdoped YBa$_{2}$Cu$_{3}$O$_{6.35}$ (T$_{c}$=18 K) has been determined throughout the Brillouin zone. At low-energy the scattering forms a cone of spin excitations emanating from the antiferromagnetic (0.5, 0.5) wave vector with an acoustic velocity similar to that of insulating cuprates. At high energy transfers, below the maximum energy of 270 meV at (0.5, 0), we observe zone boundary dispersion much larger and spectral weight loss more extensive than in insulating antiferromagnets. Moreover we report phenomena not found in insulators, an overall lowering of the zone-boundary energies and a large damping of $\sim$ 100 meV of the spin excitations at high-energies. The energy above which the damping occurs coincides approximately with the gap determined from transport measurements. We propose that as the energy is raised the spin excitations encounter an extra channel of decay into particle-hole pairs of a continuum that we associate with the pseudogap.

cond-mat.supr-con↗

arXiv2007

Quantum phase transitions in magnetism and superconductivity: emergent spin topology seen with neutrons

Magnetic spins and charges interact strongly in high-temperature superconductors. New physics emerges as layers of copper oxide are tuned towards the boundary of the superconducting phase. As the pseudogap increases the characteristic spin excitation energy decreases. We show that our well-annealed YBa2Cu3O6+x (YBCO6+x) single crystals are orthorhombic and superconducting but not antiferromagnetically ordered. Near the critical concentration for superconductivity for x = 0.35 the spins fluctuate on two energy scales, one a relaxational spin response at ~2 meV and the other a slow central mode that is resolution-limited in energy (<0.08 meV) but broad in momentum. The gradual formation on cooling of a central mode over a range of momenta suggests that the spin ground state from which coherent superconducting pairing emerges may be quantum disordered. We show that YBCO6.35 adopts a homogeneous state that consists of highly-organized frozen sub-critical three-dimensional spin correlations. The continuous spin evolution indicates that a single quantum state occurs in contrast to claims from site-based probes that lightly doped YBCO undergoes a transition to antiferromagnetic Bragg order followed by a sharp transition to a cluster glass phase. For x = 0.35, where Tc = 18 K is reduced to 1/5 of Tcmax, the spin ground state is reached without a sharp transition and consists of short correlations extending over only 8 Angstrom between cells and 42 Angstrom within the planes. Polarized neutrons show the angular spin distribution to be isotropic unlike the AF insulator. Since moment is conserved we interpret this as evidence for hole-induced spin rotations rather than decay.

cond-mat.supr-con↗

arXiv2006

The Structural Phase Transition of the Relaxor Ferroelectric 68%PbMg1/3Nb2/3O3-32%PbTiO3

Neutron scattering techniques have been used to study the relaxor ferroelectric 0.68PbMg1/3Nb2/3O3-0.32PbTiO3 denoted in this paper as 0.68PMN-0.32PT. On cooling, these relaxor ferroelectrics have a long-range ordered ferroelectric phase and the composition is close to that at which the ferroelectric structure changes from rhombohedral to tetragonal. It was found that above the Burns temperature of about 600K, the transverse optic mode and the transverse acoustic mode are strongly coupled and a model was used to describe this coupling that gave similar parameters to those obtained for the coupling in PMN. Below the Burns temperature additional quasi-elastic scattering was found which increased in intensity as the sample was cooled down to the ferroelectric transition temperature but then decreased in intensity. This behaviour is similar to that found in PMN. This scattering is associated with the dynamic polar nano-regions that occur below the Burns temperature. In addition to this scattering a strictly elastic resolution limited peak was observed that was much weaker than the corresponding peak in pure PMN and which decreased in intensity on cooling below the ferroelectric phase whereas for PMN, which does not have a long-range ordered ferroelectric phase, the intensity of this component increased monotonically as the sample was cooled. The results of our study are compared with the recent measurements of Stock et al. [PRB 73 064107] who studied 0.4PMN-0.6PT. The results are qualitatively consistent with the random field model developed to describe the scattering from PMN.

cond-mat.mtrl-sci↗

arXiv2005

Two-magnon excitations observed by neutron scattering in the two-dimensional spin-5/2 Heisenberg antiferromagnet Rb2MnF4

The low-temperature magnetic excitations of the two-dimensional spin-5/2 square-lattice Heisenberg antiferromagnet Rb2MnF4 have been probed using pulsed inelastic neutron scattering. In addition to dominant sharp peaks identified with one-magnon excitations, a relatively weak continuum scattering is also observed at higher energies. This is attributed to neutron scattering by pairs of magnons and the observed intensities are consistent with predictions of spin wave theory.

cond-mat.str-el↗

arXiv2004

From incommensurate to dispersive spin-fluctuations: The high-energy inelastic spectrum in superconducting YBa2Cu3O6.5

We have investigated the spin fluctuations at energy transfers up to ~110 meV, well above the resonance energy (33 meV) in the YBa2Cu3O6.5 ortho-II superconductor using neutron time-of-flight and triple-axis techniques. The spectrum at high energies differs from the low-energy incommensurate modulations previously reported where the incommensurate wave vector is largely independent of energy. Well above the resonance the peak of the spin response lies at wave vectors that increase with energy. Within error the excitations at all energies above the resonance are best described by a ring around the (pi, pi) position. The isotropic wave-vector pattern differs from a recently reported square pattern in different but related systems. The spin spectral weight at high-energies is similar to that in the insulator but the characteristic velocity is ~40% lower. We introduce a method of extracting the acoustic and optic weights at all energies from time-of-flight data. We find that the optic spectral weight extends to surprisingly low-energies of ~25 meV, and infer that the bilayer spin correlations weaken with increase in hole doping. When the low-energy optic excitations are taken into account we measure the total integrated weight around (pi, pi), for energies below 120 meV, to agree with that expected from the insulator. As a qualitative guide, we compare spin-wave calculations for an ordered and a disordered stripe model and describe the inadequacy of this and other stripe models for the high-energy fluctuations.

cond-mat.supr-con↗