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Optimizing the performance of magnetocaloric materials is facilitated by understanding the thermomagnetic transitions they undergo, including the order of these transitions and their strength. Those exhibiting strong first-order phase transitions (FOPT) are accompanied by large heating and cooling responses but with relatively small cyclic responses, while materials with second-order (SOPT) character exhibit moderate heating and cooling responses. However, the lack of hysteresis could partially compensate for the lower magnitudes with a more cyclic response. One way to effectively maximize the cyclic response, combining the advantages of FOPT and SOPT, is to fine tune the transition towards the borderline of FOPT-SOPT, which can minimize hysteresis. For the well-known La(Fe,Si)13 family, it is challenging to identify and/or evaluate the critical point where FOPT crossovers to SOPT based on conventional techniques. To address these ambiguities, in this work, we apply the field dependence exponent n criteria to a series of lowly hysteretic and high-performance La(Fe,Mn,Si)13H magnetocaloric materials with compositions close to the critical one. Even if the sample with the lowest hysteresis resembles characteristics of SOPT, it is evidently identified as undergoing FOPT from the n criteria: (1) existence of n > 2 overshoot and (2) n at the transition temperature, ntransition, is 0.37. This proximity to the critical composition (ntransition=0.4) further explains the low hysteresis observed. This FOPT character of the series is confirmed by temperature-dependent 57Fe Mössbauer spectrometry studies, fitting the hyperfine field to the Bean-Rodbell model instead of the usual Brillouin function. As it is a zero-field method, the confirmation by Mössbauer spectrometry gives further strength to the n-criterion.

In this study, we experimentally investigated quaternary Heusler alloys Co2−xVxFeGe with 0≤x≤1 prepared by arc melting and annealing, and showed that they are promising candidates for spintronics applications. Single phase microstructures were observed for V compositions from x=0.25 to x=0.625. Other V concentrations were multi-phased. All single phase samples had a face centered cubic crystal structure with a lattice constant that increased linearly with the V concentration. The low-temperature saturation magnetic moments were shown to obey the Slater–Pauling rule of thumb for half-metals, which is a prerequisite for half metallicity. All alloys had high Curie temperatures, which scaled linearly with the saturation magnetic moment, thereby facilitating applications at room temperature and above. Electrical transport measurements were performed to elucidate the electronic structures of the alloys. The temperature dependence of the electrical resistivity was analyzed and discussed in the framework of the two-current conduction model by considering the existence of an energy gap in the electronic spectrum around the Fermi level of the spin down sub-band. High mechanical hardness values were also observed.

In most cases, substitution studies that aim to optimize magnetic properties are performed at the magnetic atomic site. However, in the case of MnB, magnetic substitutions at the Mn site significantly decrease the once promising magnetocaloric and magnetic properties. This study employs computationally directed search to optimize the magnetocaloric properties of MnB where partial substitutions of boron atoms (Mn50B50−x Si x and Mn50B50−x Ge x where x = 3.125, 6.25, and 12.5) reveal new compounds with a greater magnetocaloric effect than pure MnB at the same Curie temperature. These new compounds were obtained by arc melting the pure elements and further characterized. The computationally driven screening process is based on density functional theory calculations that do not require large databases of known compounds. This work demonstrates that using simple computational screening procedures to search for new magnetocaloric materials with improved properties can be done quickly, cost-effectively, and while maintaining reliability.

Magnetocaloric refrigeration has remained a promising alternative to conventional refrigeration for the last few decades. The delay in reaching the market is significantly based on materials' related issues, such as hysteresis/reversibility, mechanical stability, or formability. This perspective paper shows the current trends in magnetocaloric materials research, highlighting the families of alloys and compounds that are gaining attention in the recent years. It also includes an overview of novel approaches that can be used to analyze these properties that could improve the applicability of magnetocaloric materials.

RENiX2 compounds, where RE = rare-earth element and X = p-block element, have been highly regarded for cryogenic magnetocaloric applications. Depending on the elements, they can crystallize in CeNiSi2-type, NdNiGa2-type, or MgCuAl2-type crystal structures, showing different types of magnetic ordering and thus affect their magnetic properties. Regarding the magnetocaloric effect, MgCuAl2-type aluminides show larger values than those of the CeNiSi2-type silicides and the NdNiGa2-type gallides due to the favored ferromagnetic ground state. However, RENiGa2 gallides can crystallize in either NdNiGa2- or MgCuAl2-type structures depending on the RE element. In this work, we select heavy RE (HRE) elements for exploring the microstructure, magnetic ordering and magnetocaloric performance of HRENiGa2 (HRE = Dy, Ho or Er) gallides. They all crystallize in the desired MgCuAl2-type crystal structure which undergoes a second-order transition from ferro- to para-magnetic state with increasing temperature. The maximum isothermal entropy change (∣∆Sisomax∣) values are 6.2, 10.4, and 11.4 J kg−1 K−1 (0–5 T) for DyNiGa2, HoNiGa2, and ErNiGa2, respectively, which are comparable to many recently reported cryogenic magnetocaloric materials. Particularly, the excellent magnetocaloric properties of HoNiGa2 and ErNiGa2 compounds, including their composite, fall in the temperature range that enables them for the in-demand hydrogen liquefaction systems.