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The kinetic arrest observed in the parent Gd5Ge4 gradually vanishes when a small fraction (x = 0.025, 0.05 and 0.10) of Gd is replaced by Sc in (Gd1−xScx)5Ge4, and the magnetic ground state changes from antiferromagnetic (AFM) to ferromagnetic (FM). A first order phase transition coupled with the FM-AFM transition occurs at TC = 41 K for x = 0.05 and at TC = 53 K for x = 0.10 during heating in applied magnetic field of 1 kOe, and the thermal hysteresis is near 10 K. The first-order magnetic transition is coupled with the structural Sm5Ge4-type to Gd5Si4-type transformation. The magnetization measured as a function of applied magnetic field shows sharp metamagnetic-like behavior. At the same time, the AFM to paramagnetic transition in (Gd1−xScx)5Ge4 with x = 0.10, is uncharacteristically broad indicating development of strong short-range AFM correlations above the Neel temperature. Comparison of the magnetization data of bulk, powdered, and metal-varnish composite samples of (Gd0.95Sc0.05)5Ge4 shows that mechanical grinding and fabrication of a composite have little effect on the temperature of the first-order transformation, but short-range ordering and AFM/FM ratio below TC are surprisingly strongly affected.

Magnetic and magnetocaloric properties of H o 1 - x D y x A l 2 compounds with x = 0 , 0.05 , 0.10 , 0.15 , 0.25 and 0.50 , modelled using a Hamiltonian that includes the exchange interactions between Ho-Dy, Ho-Ho and Dy-Dy ions in addition to the crystalline electric field and the Zeeman effects, have been compared with those determined experimentally. In order to reproduce experimentally observed global ferromagnetic ordering temperatures and spin reorientation transition temperatures as xDy varies, the exchange interactions between Ho-Dy and Ho-Ho were set as free parameters and adjusted to match the experimental results. We demonstrate that heat capacity of polycrystalline materials in non-zero magnetic fields can be satisfactory reproduced by using the average of multiple magnetic field directions with respect to the crystallographic coordinate system, while reasonably good agreement between experimentally determined and theoretically predicted magnetocaloric effects can be achieved considering an average of only three field directions.

Conventional magnetometry is irreplaceable in evaluating bulk magnetization of materials over broad temperature and field ranges. The technique is also effective in quantifying hysteresis that may be associated with magnetic and structural phase transitions that occur during the magnetizing/demagnetizing cycling, and the derived magnetic field-induced isothermal entropy change – one of the most important properties in the field of magnetocalorics. Both systematic and random errors present during the measurements of magnetization, however, may lead to erroneous conclusions. Using two well-known materials – elemental Gd and intermetallic Gd5Si2Ge2 as examples, we consider best practices in performing reliable and rapid magnetization measurements for proper characterization of magnetocaloric properties.

Using first-principles calculations, based on disordered local moment theory, combined with the self-interaction corrected local spin density approximation, we study magnetic interactions in GdX intermetallics for X = Cu, Zn, Ga, Cd, and Mg. Our predicted magnetic orders and ordering temperatures both at zero and other pressures agree well with experiments including the large increase in the Curie temperature of GdCd under pressure that is shown by our own experimental measurements. From our results it emerges that the Ruderman-Kittel-Kasuya-Yosida interaction on its own can not explain the observed behaviour under pressure, and that the magnetic ordering mechanism is strongly influenced by the occupations of both Gd and anion d -bands.

Rare-earth anti-perovskites with oxygen are an interesting magnetic materials family at the boundary between intermetallics and oxides, they however remain largely unexplored. Here, magnetic and heat capacity investigations, as well as density functional theory (DFT) calculations, were carried out on SnOEu3. At low magnetic field (B ≤ 0.5 T), a Neel temperature separates antiferromagnetic and paramagnetic phases at 31 K. When applying higher magnetic field below the Neel temperature, successive transformations toward a ferromagnetic state via a number of intermediate canted magnetic structures are observed and are associated with only modest latent heat and transition entropy. High-pressure magnetic measurements confirm the stable divalent state of Eu up to 1.05 GPa. A direct magnetocaloric effect progressively increases with applied magnetic field above the Neel temperature, reaching −16 J kg–1 K−1 for ΔB = 7 T. On the other hand, the inverse magnetocaloric effect of the field-induced transition below TN saturates at ~+5 J kg−1 K−1. DFT calculations support magnetic instabilities observed experimentally in SnOEu3 and reveal an unusual exchange mechanism and band topology near the Fermi level.

We have investigated the effects of quenching rate on the thermal dependence of the magnetic entropy change ΔSM(T) and the magnetic field induced hysteresis loss through the antiferromagnetic (AFM) ↔ ferromagnetic (FM) transformation in bulk Fe49Rh51. Two nearly identical square-prism-shaped samples were subjected to two different temperature cooling regimes; one was rapidly quenched (FQ) in iced-water and another slow cooled (SC) to room temperature at a cooling rate of 2 K/min. The temperature of the AFM ↔ FM transition is similar for both samples, but the FQ sample shows much sharper temperature- and magnetic field-induced magnetization change; in addition, the total magnetization change is 14% larger. In FQ material, the magnetocaloric effect, i.e., ΔSM(T) quickly approaches saturation above 1 T and shows a large peak value at 2 T (13.9 versus 8.9 Jkg−1 K−1 in SC material), but a larger average hysteresis loss FWHM in the temperature range coinciding with of the full-width at half-maximum of the ΔSM(T) curve.