Andrew Boothroyd

Abstract:

We have investigated the optimum conditions for the growth of Na xCoO2 single crystals by the optical floating-zone technique. A significant reduction in Na loss, was achieved by using a high-pressure growth atmosphere. A high-pressure oxygen-rich atmosphere during crystal growth was found to reduce the presence of CO3O4 impurity phase in the grown crystal. The magnetic properties of powder and single crystal samples were measured by superconducting quantum interference device (SQUID) magnetometry and found to vary according to the preparation conditions. © 2004 Elsevier B.V. All rights reserved.

Abstract:

In this paper we report studies of the charge stripe ordering using high resolution x-ray scattering in the nickelate system La2-xSr xNiO4 with doping levels of x=0.33, x=0.30, and x=0.275. The charge stripes for all doping levels were found to be two dimensional in nature with a high degree of correlation in the a-b plane. The in-plane inverse correlation length in the lower doped systems was greater than that in the x=0.33 system and is greatest for x=0.275, consistent with the stripes becoming less correlated as the doping level is decreased from x=0.33. However, the charge ordering in the x=0.33 system was observed to be more two dimensional in nature with a greater inverse correlation length between planes. The interaction between the lattice and charge order was observed to stabilize the charge ordering, even in the absence of spin ordering. In the x=0.30 and x=0.275 systems no long-range charge order could exist without the presence of the magnetic order. In both systems the charge stripes were incommensurate and on heating the incommensurability increased towards the stable ε=0.33 value as the stripes gained thermal energy to overcome the Coulombic repulsion. In all these systems the integrated intensity of the stripe reflections showed a clear difference in behavior from previous neutron studies with an initial increase in the integrated intensity as the temperature was increased, which was not found in the neutron studies.

Abstract:

We report neutron diffraction data on single crystal PrO2 which reveal a cooperative Jahn-Teller distortion at TD=120±2 K. Below this temperature an internal distortion of the oxygen sublattice causes the unit cell of the crystallographic structure to become doubled along one crystal axis. We discuss several possible models for this structure. The antiferromagnetic structure below TN=13.5 K is found to consist of two components, one of which shares the same doubled unit cell as the distorted crystallographic structure. We also present measurements of the magnetic susceptibility, the specific heat capacity, and the electrical conductivity of PrO2. The susceptibility data show an anomaly at a temperature close to TD. From the specific heat capacity data we deduce that the ground state is doubly degenerate, consistent with a distortion of the cubic local symmetry. We discuss possible mechanisms for this. The conductivity shows an activated behavior with an activation energy Ea=0.262±0.003 eV.

Abstract:

We present a neutron diffraction study of the magnetic structure of single crystal PrO2 under applied fields of 0-6 T. As the field is increased, changes are observed in the magnetic Bragg intensities. These changes are found to be irreversible when the field is reduced, but the original intensities can be recovered by heating to T> 122 K, then recooling in zero field. The antiferromagnetic ordering temperature TN=13.5 K and the magnetic periodicity are unaffected by the applied field. We also report measurements of the magnetic susceptibility of single crystal PrO2 under applied fields of 0-7 T. These show strong anisotropy, as well as an anomaly at T=122±2 K, which coincides with the temperature T D=120±2 K, at which a structural distortion occurs. For fields applied along the [100] direction the susceptibility increases irreversibly with field in the temperature range TND. However, for fields along [110] the susceptibility is independent of field in this range. We propose structural domain alignment, which strongly influences the formation of magnetic domains below TN, as the mechanism behind these changes.

Abstract:

Magnetic order has been investigated in stripe-ordered La 2-xSrxNiO4 (x=0.275,0.37,0.4) by dc magnetization and by polarized- and unpolarized-neutron diffraction. In the magnetically ordered phase, all three compositions exhibit a magnetic transition consistent with a spin reorientation in the ab plane. For x=0.37, the spin axes rotate from an angle of 37.7°±0.3° to the stripe direction at 71 K, to 52.3°±0.20 at 2 K. The x=0.275 and 0.4 compounds were found to undergo a similar spin reorientation. A spin reorientation has now been observed to occur for five different doping levels in the range of 0.275≤x≤0.5, suggesting that this spin transition is an intrinsic property of the stripe phase.