Andrew Boothroyd

Abstract:

The magnetic properties of the S=1/2 two-dimensional square-lattice antiferromagnets Sr2NiO3X (X=Cl, F) with the trivalent nickel ions in a low-spin state were studied by magnetic susceptibility, heat capacity, neutron powder diffraction, high-field electron spin resonance (ESR), muon spin rotation and relaxation (μ+SR) measurements, and density functional theory (DFT) calculations. Both oxyhalides are isostructural to an ideal quantum square-lattice antiferromagnet Sr2CuO2Cl2, but the chlorine/fluorine anion exclusively occupies an apical site in an ordered/disordered manner with an oxygen anion, resulting in the formation of highly distorted NiO5X octahedra with an off-center nickel ion. Magnetic susceptibility measurements revealed a remarkable difference between these two compounds: the magnetic susceptibility of Sr2NiO3Cl exhibited a broad maximum at approximately 35 K, which is typical of low-dimensional antiferromagnetic behavior. In contrast, the magnetic susceptibility of Sr2NiO3F exhibited spin-glass-like behavior below 12 K. No anomaly associated with long-range magnetic ordering was observed in the heat capacity, ESR, and neutron powder diffraction experiments. However, μ+SR measurements revealed the emergence of a static magnetic ordered state below TN=28K in Sr2NiO3Cl and a short-range magnetic state below TN=18K in Sr2NiO3F. The DFT calculations suggested that the unpaired electron occupied a d3z2-r2 orbital, and ferromagnetic couplings between the nearest-neighbor nickel spins were energetically favored. The mechanism of ferromagnetic superexchange interactions and the reason for the difference between the magnetic ground states in these nickel oxyhalides are discussed.

Abstract:

According to previous theoretical work, the binary oxide CuO can become a room temperature multiferroic via tuning of the superexchange interactions by application of pressure. Thus far, however, there has been no experimental evidence for the predicted room-temperature multiferroicity. Here, we show by neutron diffraction that the multiferroic phase in CuO reaches 295 K with the application of 18.5 GPa pressure. We also develop a spin Hamiltonian based on density functional theory and employing superexchange theory for the magnetic interactions, which can reproduce the experimental results. The present study provides a stimulus to develop room-temperature multiferroic materials by alternative methods based on existing low temperature compounds, such as epitaxial strain, for tunable multifunctional devices and memory applications.

Abstract:

Co3Sn2S2 has recently been predicted to be a Weyl semimetal in which magnetic order is key to its behavior as a topological material. Here, we report unpolarized neutron diffraction and spherical neutron polarimetry measurements, supported by magnetization and transport data, which probe the magnetic order in Co3Sn2S2 below TC=177 K. The results are fully consistent with ferromagnetic order in which the spins on the Co atoms point along the crystal c axis, although we cannot rule out some canting of the spins. We find no evidence for a type of long-ranged (k=0) in-plane 120° antiferromagnetic order which had previously been considered as a secondary phase present at temperatures between ∼90 K and TC. A discontinuous change in bulk properties and neutron polarization observed at T=125 K when samples are cooled in a field and measured on warming is found to be due to a sudden reduction in ferromagnetic domain size. Our results lend support to the theoretical predictions that Co3Sn2S2 is a magnetic Weyl semimetal.

Abstract:

In this work, we explore experimentally and theoretically the spectrum of magnetic excitations of the Fe3+ and Yb3+ ions in ytterbium iron garnet (Yb3Fe5O12). We present a complete description of the crystal-field splitting of the 4f states of Yb3+, including the effect of the exchange field generated by the magnetically ordered Fe subsystem. We also consider a further effect of the Fe-Yb exchange interaction, which is to hybridize the Yb crystal field excitations with the Fe spin-wave modes at positions in the Brillouin zone where the two types of excitations cross. We present detailed measurements of these hybridized excitations, and we propose a framework that can be used in the quantitative analysis of the coupled spectra in terms of the anisotropic 4f-3d exchange interaction.