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We investigate the properties of ${\mathrm{CuVOF}}_4{\left({\mathrm{H}}_2\mathrm{O}\right)}_6·{\mathrm{H}}_2\mathrm{O}$, in which two different spin species, Cu(II) and V(IV), form antiferromagnetic spin-1/2 dimers with weak interdimer coupling provided via hydrogen bonding. Using radio-frequency susceptometry and electron-spin resonance (ESR), we show how the temperature-magnetic field spin-dimer phase diagram evolves as a function of applied hydrostatic pressure and correlate this with pressure-induced changes to the crystal structure. These results, coupled with pressure-tuned DFT calculations, confirm the prior prediction that the primary exchange interaction is mediated via an unusual mechanism in which the V(IV) ions provide considerable spin density to the oxygen that joins the two spins in each dimer and which lies along the Jahn-Teller axis of the Cu(II) ion. In addition, the dissimilarity in the spins that make up each dimer unit leads to a nonlinear field dependence of the electronic energy levels as detected in the ESR measurements. 

Materials composed of spin-1 antiferromagnetic (AFM) chains are known to adopt complex ground states that are sensitive to the single-ion-anisotropy (SIA) energy ( $D$), and intrachain ( $J_0$) and interchain ( $J_{1,2}^{\prime }$) exchange energy scales. While theoretical and experimental studies have extended this model to include various other energy scales, the effect of the lack of a common SIA axis is not well explored. Here we investigate the magnetic properties of $\mathrm{Ni}\left(\mathrm{pyrimidine}\right){\left({\mathrm{H}}_2\mathrm{O}\right)}_2{\left({\mathrm{NO}}_3\right)}_2$, a chain compound where the tilting of Ni octahedra leads to a twofold alternation of the easy-axis directions along the chain. Muon-spin relaxation measurements indicate a transition to long-range order at $T_{\text{N}}=2.3\mathrm{K}$and the magnetic structure is initially determined to be antiferromagnetic and collinear using elastic neutron diffraction experiments. Inelastic neutron scattering measurements were used to find $J_0=5.107\left(7\right)\mathrm{K}, D=2.79\left(1\right)\mathrm{K},J_1^{\prime }=0.00\left(5\right)\mathrm{K}, J_2^{\prime }=0.18\left(3\right)\mathrm{K}$, and a rhombic anisotropy energy $E=0.19\left(9\right)\mathrm{K}$. Mean-field modeling reveals that the ground state structure hosts spin canting of $\varphi \approx 6.5^{\circ }$, which is not detectable above the noise floor of the elastic neutron diffraction data. Monte Carlo simulation of the powder-averaged magnetization, $M\left(H\right)$, is then used to confirm these Hamiltonian parameters, while single-crystal $M\left(H\right)$simulations provide insight into features observed in the data. Published by the American Physical Society2025 

We investigate the magnetic properties of $S=1$antiferromagnetic diamond-lattice, $\mathrm{Ni}{X}_2{\left(\mathrm{pyrimidine}\right)}_2$ $(X=\mathrm{Cl}, \mathrm{Br})$, hosting a single-ion anisotropy (SIA) orientation which alternates between neighboring sites. Through neutron diffraction measurements of the $X=\mathrm{Cl}$compound, the ordered state spins are found to align collinearly along a pseudo-easy axis, a unique direction created by the intersection of two easy planes. Similarities in the magnetization, exhibiting spin-flop transitions, and the magnetic susceptibility in the two compounds imply that the same magnetic structure and a pseudo-easy axis is also present for $X=\mathrm{Br}$. We estimate the Hamiltonian parameters by combining analytical calculations and Monte Carlo (MC) simulations of the spin-flop and saturation field. The MC simulations also reveal that the spin-flop transition occurs when the applied field is parallel to the pseudo-easy axis. Contrary to conventional easy-axis systems, there exist field directions perpendicular to the pseudo-easy axis for which the magnetic saturation is approached asymptotically and no symmetry-breaking phase transition is observed at finite fields. Published by the American Physical Society2024 

We present the magnetic and structural properties of [Cu(pyrazine)0.5(glycine)]ClO4 under applied pressure. As previously reported, at ambient pressure this material consists of quasi-two-dimensional layers of weakly coupled antiferromagnetic dimers which undergo Bose-Einstein condensation of triplet excitations between two magnetic field-induced quantum critical points (QCPs). The molecular building blocks from which the compound is constructed give rise to exchange strengths that are considerably lower than those found in other S = 1/2 dimer materials, which allows us to determine the pressure evolution of the entire field-temperature magnetic phase diagram using radio-frequency magnetometry. We find that a distinct phase emerges above the upper field-induced transition at elevated pressures and also show that an additional QCP is induced at zero field at a critical pressure of pc = 15.7(5) kbar. Pressure-dependent single-crystal x-ray diffraction and density functional theory calculations indicate that this QCP arises primarily from a dimensional crossover driven by an increase in the interdimer interactions between the planes. While the effect of quantum fluctuations on the lower field-induced transition is enhanced with applied pressure, quantum Monte Carlo calculations suggest that this alone cannot explain an unconventional asymmetry that develops in the phase diagram. 

Abstract CeOs 4 Sb 12 , a member of the skutterudite family, has an unusual semimetallic low-temperature L -phase that inhabits a wedge-like area of the field H —temperature T phase diagram. We have conducted measurements of electrical transport and megahertz conductivity on CeOs 4 Sb 12 single crystals under pressures of up to 3 GPa and in high magnetic fields of up to 41 T to investigate the influence of pressure on the different H – T phase boundaries. While the high-temperature valence transition between the metallic H -phase and the L -phase is shifted to higher T by pressures of the order of 1 GPa, we observed only a marginal suppression of the S -phase that is found below 1 K for pressures of up to 1.91 GPa. High-field quantum oscillations have been observed for pressures up to 3.0 GPa and the Fermi surface of the high-field side of the H -phase is found to show a surprising decrease in size with increasing pressure, implying a change in electronic structure rather than a mere contraction of lattice parameters. We evaluate the field-dependence of the effective masses for different pressures and also reflect on the sample dependence of some of the properties of CeOs 4 Sb 12 which appears to be limited to the low-field region.