X-ray and neutron scattering

Abstract:

The rational design of disordered frameworks is an appealing route to target functional materials. However, intentional realisation of such materials relies on our ability to readily characterise and quantify structural disorder. Here, we use multivariate analysis of pair distribution functions to fingerprint and quantify the disorder within a series of compositionally identical metal-organic frameworks, possessing different crystalline, disordered, and amorphous structures. We find this approach can provide powerful insight into the kinetics and mechanism of structural collapse that links these materials. Our methodology is also extended to a very different system, namely the melting of a zeolitic imidazolate framework, to demonstrate the potential generality of this approach across many areas of disordered structural chemistry.

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.

Abstract:

CeRh 3 Si 2 has been reported to exhibit metamagnetic transitions below 5 K, a giant crystal field splitting, and anisotropic magnetic properties from single crystal magnetization and heat capacity measurements. Here we report results of neutron and x-ray scattering studies of the magnetic structure and crystal-field excitations to further understand the magnetism of this compound. Inelastic neutron scattering and resonant inelastic x-ray scattering reveal a J z = 1 / 2 ground state for Ce when considering the crystallographic a direction as quantization axis, thus explaining the anisotropy of the static susceptibility. Furthermore, we find a total splitting of 78 meV for the J = 5 / 2 multiplet. The neutron diffraction study in zero field reveals that, on cooling from the paramagnetic state, the system first orders at T N 1 = 4.7 K in a longitudinal spin density wave with ordered Ce moments along the b axis (i.e., the [0 1 0] crystal direction) and an incommensurate propagation vector k = ( 0 , 0.43 , 0 ). Below the lower-temperature transition T N 2 = 4.48 K , the propagation vector locks to the commensurate value k = ( 0 , 0.5 , 0 ) , with a so-called lock-in transition. Our neutron diffraction study in applied magnetic field H ∥ b axis shows a change in the commensurate propagation vector and development of a ferromagnetic component at H = 3 kOe , followed by a series of transitions before the fully field-induced ferromagnetic phase is reached at H = 7 kOe . This explains the nature of the steps previously reported in field-dependent magnetization measurements. A very similar behavior is also observed for the H ∥ [0 1 1] crystal direction.