No abstract

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 σ(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.

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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±0.009 eV, 1.84±0.03, and 2.30±0.15 eV. These were parameterized within a weak crystal field scheme with an intra-orbital exchange of J(dd)=1.3 ± 0.2 eV and a crystal field splitting 10Dq=0.94 ± 0.10 eV. A reduced spinorbit coupling of λ=-0.016± 0.003 eV is derived from dilute samples of Mg0.97Co0.03O, 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 A2 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.

The industrially important interaction of methanol with an eta-alumina catalyst has been investigated by a combination of infrared spectroscopy (diffuse reflectance and transmission) and inelastic neutron scattering (INS) spectroscopy. The infrared and INS spectra together show that chemisorbed methoxy is the only surface species present. Confirmation of the assignments was provided by a periodic DFT calculation of methoxy on eta-alumina (110). The thermal conversion of adsorbed methoxy groups to form dimethylether was also followed by INS, with DFT calculations assisting assignments. An intense feature about 2600 cm(-1) was observed in the diffuse reflectance spectrum. This band is poorly described in the extensive literature on the alumina/methanol adsorption system and its observation raised the possibility of a new surface species existing on this particular catalyst surface. INS measurements established that the 2600 cm(-1) feature could be assigned to a combination band of the methyl rock with the methyl deformation modes. This assignment was reinforced by an analysis of the neutron scattering intensity at a particular energy as a function of momentum transfer, which confirmed this particular adsorbed methoxy feature to arise from a second order transition. Similar behaviour was observed in the model compound Al(OCH3)3. The anomalous infrared intensity of the 2600 cm(-1) peak in the diffuse reflectance spectrum is a consequence of the different absorption coefficients of the C-H stretch and the combination mode. The implications for catalyst studies are discussed.

We have measured the spin fluctuations in the YBa 2 Cu 3 O 6.5 ͑YBCO 6.5 , T c =59 K͒ superconductor at highenergy transfers above ϳ100 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 ϳ100 meV similar to that observed above ϳ200 meV in the YBCO 6.35 ͑T c =18 K͒ superconductor as the spin waves approach the zone boundary. We attribute this highenergy 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.

The S=2 anisotropic triangular lattice alpha-NaMnO2 is studied by neutron inelastic scattering. Antiferromagnetic order occurs at T< or =45 K with opening of a spin gap. The spectral weight of the magnetic dynamics above the gap (Delta approximately equal to 7.5 meV) has been analyzed by the single-mode approximation. Excellent agreement with the experiment is achieved when a dominant exchange interaction (|J|/k(B) approximately 73 K), along the monoclinic b axis and a sizable easy-axis magnetic anisotropy (|D|/k(B) approximately 3 K) are considered. Despite earlier suggestions for two-dimensional spin interactions, the dynamics illustrate strongly coupled antiferromagnetic S=2 chains and cancellation of the interchain exchange due to the lattice topology. alpha-NaMnO2 therefore represents a model system where the geometric frustration is resolved through the lowering of the dimensionality of the spin interactions.

An iron based Fischer-Tropsch synthesis catalyst is evaluated using CO hydrogenation at ambient pressure as a test reaction and is characterised by a combination of inelastic neutron scattering (INS), powder X-ray diffraction, temperature-programmed oxidation, Raman scattering, and transmission electron microscopy. The INS spectrum of the as-prepared bulk iron oxide pre-catalyst (hematite, α-Fe2O3) is distinguished by a relatively intense band at 810 cm(-1), which has previously been tentatively assigned as a magnon (spinon) feature. An analysis of the neutron scattering intensity of this band as a function of momentum transfer unambiguously confirms this assignment. Post-reaction, the spinon feature disappears and the INS spectrum is characterised by the presence of a hydrocarbonaceous overlayer. A role for the application of INS in magnetic characterisation of iron based FTS catalysts is briefly considered.