X-ray and neutron scattering

Abstract:

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 models of the excitation spectrum fail 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.

Abstract:

Using resonant magnetic x-ray scattering we address the unresolved nature of the magnetic groundstate and the low-energy effective Hamiltonian of Sm2Ir2O7, 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 DzyaloshinskiiMoriya interaction (D = 4.9(3) meV), which provides a consistent description of the magnetic order and excitations. In establishing that Sm2Ir2O7 has the requisite inversion symmetry preserving AIAO magnetic groundstate, our results support the notion that pyrochlore iridates may host correlated Weyl semimetals.

Abstract:

Metals cannot exhibit ferroelectricity because static internal electric fields are screened by conduction electrons, but in 1965, Anderson and Blount predicted the possibility of a ferroelectric metal, in which a ferroelectric-like structural transition occurs in the metallic state. Up to now, no clear example of such a material has been identified. Here we report on a centrosymmetric (R3c) to non-centrosymmetric (R3c) transition in metallic LiOsO3 that is structurally equivalent to the ferroelectric transition of LiNbO3 (ref. 3). The transition involves a continuous shift in the mean position of Li(+) ions on cooling below 140 K. Its discovery realizes the scenario described in ref. 2, and establishes a new class of materials whose properties may differ from those of normal metals.

Abstract:

Sr2MnO2Cu3.5S3 contains mixed-valent Mn ions Mn2+/3+ in axially elongated MnO4S2 octahedra connected via apical sulfide anions to copper-deficient antifluorite-type Cu4-δS3 layers where δ ∼ 0.5. Copper deficiency is charge-compensated by oxidation of Mn 3d states resulting in mixed-valency. The compound is tetragonal in P4/mmm at ambient temperatures (a = 4.016345(1) Å, c = 11.40708(5) Å). Below 190 K, superlattice reflections in diffraction data and an increase in resistivity, signal checkerboard charge-ordering of Mn2+ and Mn3+. The superstructure approximates to a √2a × √2a × 2c expansion of the room temperature cell in space group P42/nmc. However, satellite reflections signal a (3 + 2)D incommensurate modulation of Cu site occupancies in the Cu-deficient sulfide layers coupled with displacements of the sulfur positions; overall the superstructure below 190 K requires description in superspace group P42/nmc(a,0,0)0000(0,a,0)00s0. Analysis of total scattering measurements along with pair distribution functions supports the charge-ordered low temperature model and reveals local order of distinct Mn sites within the higher-temperature charge-disordered regime. Below TN = 27 K, long-range magnetic ordering is A-type antiferromagnetic with distinct moments for Mn2+ and Mn3+ ions directed perpendicular to the MnO2 planes and ordered ferromagnetically. Long-range antiferromagnetic order results from interlayer antiferromagnetic coupling. A metamagnetic transition at 1.1 T corresponds to a change to long-range interlayer ferromagnetic ordering via a spin-reorientation of magnetic moments and is associated with a slight decrease in the charge separation between the Mn sublattices, consistent with observations on mixed-valent perovskite and Ruddlesden-Popper-type oxide manganites.