arXiv subjects

Helen Y. Playford

Publications and source records attributed to Helen Y. Playford.

4 recordsLinked to original sources

arXiv2026

A comparison of the spin-phonon behaviour of Fe$_2$P-based magnetocaloric materials

Magnetic refrigeration can provide an environmentally friendly technology to reduce significantly the energy consumption of cooling devices. To retain the sustainability of the device, all parts must be made from abundant materials, excluding e.g. rare earth elements. As such, materials based on Fe$_2$P have shown great potential for magnetocaloric devices. In this study, Fe$_2$P and FeMnP$_{0.55}$Si$_{0.45}$, have been studied using magnetometry, neutron scattering and theoretical modelling with the aim to understand the ferromagnetic transition, related to the magnetocaloric effect. Analysis of the diffraction data of Fe$_2$P showed that it is the Fe$_{3g}$-site that drives the magnetic transition as the Fe$_{3f}$ does not have any magnetic contribution at the magnetic transition temperature. For FeMnP$_{0.55}$Si$_{0.45}$, the magnetic transition is more gradual, on both sites, with coexistence of the para- and ferromagnetic phases close to the magnetic transition. The temperature dependent magnetic structure behaviour are well in agreement with our first principles calculations. Both Fe$_2$P and FeMnP$_{0.55}$Si$_{0.45}$ showed two distinct regions, at different length scales, in their S(\textbf{Q},$ω$) spectra. The two length scales can be modelled using a different set of magnetic spin states (S), using S$\rm _{Fe}$~=~2 and S$\rm _{Mn}$~=~2.5, consistent with the ground state of the magnetic atoms. QENS at low Q (Q~\textless{}~0.5~Å) shows similar magnetic processes in both compounds with uncorrelated magnetism below the magnetic transition temperature. The uncorrelated state highlights that the magnetic anisotropy does not play a major role in the formation of the magnetic state. Furthermore, this emphasises the existence of a two part system in FeMn(P,Si)-based compounds, that drives the magnetic transition and in turn the magnetocaloric effect.

cond-mat.mtrl-sci↗

arXiv2022

Origin of the large entropy change in the molecular caloric and ferroelectric ammonium sulfate

The deceptively simple inorganic salt ammonium sulfate undergoes a ferroelectric phase transition associated with a very large entropy change and both electrocaloric and barocaloric functionality. While the structural origins of the electrical polarisation are now well established, those of the entropy change have been controversial for over fifty years. This question is resolved here using a combination of DFT phonon calculations with inelastic neutron scattering under variable temperature and pressure, supported by complementary total and quasielastic neutron scattering experiments. A simple model of the entropy in which each molecular ion is disordered across the mirror plane in the high symmetry phase, although widely used in the literature, proves to be untenable. Instead, the entropy arises from low-frequency librations of ammonium ions in this phase, with harmonic terms that are very small or even negative. These results suggest that, in the search for molecular materials with functionality derived from large entropy changes, vibrational entropy arising from broad energy minima is likely to be just as important as configurational entropy arising from crystallographic disorder.

cond-mat.mtrl-sci↗

arXiv2019

Room temperature spin-ice physics in cadmium cyanide

Spin-ices are frustrated magnets that support a particularly rich variety of emergent physics. Typically, it is the interplay of magnetic dipole interactions, spin anisotropy, and geometric frustration on the pyrochlore lattice that drives spin-ice formation. The relevant physics occurs at temperatures commensurate with the magnetic interaction strength, which for most systems is 1--5\,K. This low energy scale poses severe challenges for experimental studies of spin-ices and the practical exploitation of their unusual properties. Here, we show that non-magnetic cadmium cyanide (Cd(CN)$_2$) exhibits analogous behaviour to magnetic spin-ices, but does so on a temperature scale that is nearly two orders of magnitude greater. The electric dipole moments of cyanide ions in Cd(CN)$_2$ assume the role of magnetic pseudospins, with the difference in energy scale reflecting the increased strength of electric \emph{vs} magnetic dipolar interactions. As a result, spin-ice physics influences the structural behaviour of Cd(CN)$_2$ even at room temperature.

cond-mat.mtrl-sci↗

arXiv2016

Orbital Dimer Model for Spin-Glass State in Y$_2$Mo$_2$O$_7$

The formation of a spin glass usually requires both structural disorder and frustrated magnetic interactions. Consequently, the origin of spin-glass behaviour in Y$_2$Mo$_2$O$_7$ $-$ in which magnetic Mo$^{4+}$ ions occupy a frustrated pyrochlore lattice with minimal compositional disorder $-$ has been a longstanding question. Here, we use neutron and X-ray pair-distribution function (PDF) analysis to develop a disorder model that resolves apparent incompatibilities between previously-reported PDF, EXAFS and NMR studies and provides a new and physical mechanism for spin-glass formation. We show that Mo$^{4+}$ ions displace according to a local "2-in/2-out" rule on each Mo$_4$ tetrahedron, driven by orbital dimerisation of Jahn-Teller active Mo$^{4+}$ ions. Long-range orbital order is prevented by the macroscopic degeneracy of dimer coverings permitted by the pyrochlore lattice. Cooperative O$^{2-}$ displacements yield a distribution of Mo$-$O$-$Mo angles, which in turn introduces disorder into magnetic interactions. Our study demonstrates experimentally how frustration of atomic displacements can assume the role of compositional disorder in driving a spin-glass transition.

cond-mat.str-el↗