The phase‐down scenario of conventional refrigerants used in gas–vapor compressors and the demand for environmentally friendly and efficient cooling make the search for alternative technologies more important than ever. Magnetic refrigeration utilizing the magnetocaloric effect of magnetic materials could be that alternative. However, there are still several challenges to be overcome before having devices that are competitive with those based on the conventional gas–vapor technology. In this paper a rigorous assessment of the most relevant examples of 14 different magnetocaloric material families is presented and those are compared in terms of their adiabatic temperature and isothermal entropy change under cycling in magnetic‐field changes of 1 and 2 T, criticality aspects, and the amount of heat that they can transfer per cycle. The work is based on magnetic, direct thermometric, and calorimetric measurements made under similar conditions and in the same devices. Such a wide‐ranging study has not been carried out before. This data sets the basis for more advanced modeling and machine learning approaches in the near future.

We present phonon dispersions, element-resolved vibrational density of states (VDOS) and corresponding thermodynamic properties obtained by a combination of density functional theory (DFT) and nuclear resonant inelastic x-ray scattering (NRIXS) across the metamagnetic transition of B2 FeRh in the bulk material and thin epitaxial films. We see distinct differences in the VDOS of the antiferromagnetic (AF) and ferromagnetic (FM) phases, which provide a microscopic proof of strong spin-phonon coupling in FeRh. The FM VDOS exhibits a particular sensitivity to the slight tetragonal distortions present in epitaxial films, which is not encountered in the AF phase. This results in a notable change in lattice entropy, which is important for the comparison between thin film and bulk results. Our calculations confirm the recently reported lattice instability in the AF phase. The imaginary frequencies at the X point depend critically on the Fe magnetic moment and atomic volume. Analyzing these nonvibrational modes leads to the discovery of a stable monoclinic ground-state structure, which is robustly predicted from DFT but not verified in our thin film experiments. Specific heat, entropy, and free energy calculated within the quasiharmonic approximation suggest that the new phase is possibly suppressed because of its relatively smaller lattice entropy. In the bulk phase, lattice vibrations contribute with the same sign and in similar magnitude to the isostructural AF-FM phase transition as excitations of the electronic and magnetic subsystems demonstrating that lattice degrees of freedom need to be included in thermodynamic modeling.

Magnetic refrigeration relies on a substantial entropy change in a magnetocaloric material when a magnetic field is applied. Such entropy changes are present at first‐order magnetostructural transitions around a specific temperature at which the applied magnetic field induces a magnetostructural phase transition and causes a conventional or inverse magnetocaloric effect (MCE). First‐order magnetostructural transitions show large effects, but involve transitional hysteresis, which is a loss source that hinders the reversibility of the adiabatic temperature change ΔTad. However, reversibility is required for the efficient operation of the heat pump. Thus, it is the mastering of that hysteresis that is the key challenge to advance magnetocaloric materials. We review the origin of the large MCE and of the hysteresis in the most promising first‐order magnetocaloric materials such as Ni–Mn‐based Heusler alloys, FeRh, La(FeSi)13‐based compounds, Mn3GaC antiperovskites, and Fe2P compounds. We discuss the microscopic contributions of the entropy change, the magnetic interactions, the effect of hysteresis on the reversible MCE, and the size‐ and time‐dependence of the MCE at magnetostructural transitions.

The present study on magnetic and structural properties of Ni50Mn45Ga5 confirms that structural metastability is an inherent property of Ni50Mn50–xXx Heusler alloys with X as In, Ga, and Sn. The ternary alloy transforms during temper-annealing into a dual-phase composite alloy. The two phases are identified to be cubic L21, Ni50Mn25Ga25, and tetragonal L10 Ni50Mn50. Depending on the annealing temperature, the magnetic-proximity effect giving rise to shell-ferromagnetism has been observed when annealing is carried out under an external magnetic field. The upper and lower remanence values MR+ and MR− have the same sign even at high temperatures. Such alloys can be promising candidates for heat- and magnetic-field-resistant magnetic recording media.