Megan R. Rutherford | Searcharxiv

arXiv2026

K$_2$Co$_2$(TeO$_{3}$)$_{3}$ $\cdot$ 2.5 H$_2$O : A mineral-inspired pseudo-honeycomb cobalt dimer antiferromagnet

In recent years, magnetically-frustrated triangular and honeycomb lattice cobaltates have seen extensive study in the pursuit of a quantum spin liquid (QSL) state in a real material. In this work, we describe the hydroflux synthesis of K$_2$Co$_2$(TeO$_{3}$)$_{3}$ $\cdot$ 2.5 H$_2$O (KCoTOH), a novel zemannite-type antiferromagnet (AFM) possessing structural elements of both triangular dimer and honeycomb structural motifs. Bulk magnetometry and specific heat data support the onset of long-range AFM order below $T_\text{N}$ = 7.6(1) K, with neutron diffraction and muon spin relaxation ($μ$SR) measurements placing the majority of the ordered moment within the pseudo-honeycomb plane. We resolve three unique oscillation frequencies from the zero-field $μ$SR spectra, additionally suggesting a remarkably low level of structural disorder in as-grown KCoTOH crystals. Whereas interactions between dimerized chains of Co$^{2+}$ cations are typically observed to be negligible or ferromagnetic in nature, the largely planar ordering motif observed in KCoTOH is instead stabilized by net antiferromagnetic interactions through bridging tellurite groups. This work highlights the potential of hydroflux synthesis methods in the stabilization of magnetic materials possessing novel and potentially more frustrated lattice geometries.

cond-mat.str-el↗

arXiv2024

Impact of synthesis method on the structure and function of high entropy oxides

The term sample dependence describes the troublesome tendency of nominally equivalent samples to exhibit different physical properties. High entropy oxides (HEOs) are a class of materials where sample dependence has the potential to be particularly profound due to their inherent chemical complexity. In this work, we prepare a spinel HEO of identical nominal composition by five distinct methods, spanning a range of thermodynamic and kinetic conditions: solid state, high pressure, hydrothermal, molten salt, and combustion syntheses. By structurally characterizing these five samples across all length scales with a variety of x-ray methods, we find that while the average structure is unaltered, the samples vary significantly in their local structures and their microstructures. The most profound differences are observed at intermediate length scales, both in terms of crystallite morphology and cation homogeneity. As revealed by x-ray fluorescence microscopy ideal cation homogeneity is achieved only in the case of combustion synthesis. These structural differences in turn significantly alter the observed functional properties, which we demonstrate via characterization of their magnetic response. While ferrimagnetic order is retained across all five samples, the sharpness of the transition, the size of the saturated moment, and the coercivity all show marked variations with synthesis method. We conclude that the chemical flexibility inherent to HEOs is complemented by strong synthesis method dependence, providing another axis along which to optimize these materials for a wide range of applications.

cond-mat.mtrl-sci↗