Tailoring the cryogenic magnetism and magnetocaloric effect from Zr substitution in EuTiO₃ perovskite

Refrigeration in the liquid helium temperature range provides vital technological support for many scientific frontiers and engineering technologies. The considerable magnetocaloric effect (MCE) makes EuTiO₃ a potential candidate for magnetic refrigeration near liquid helium temperature. More interestingly, the magnetic transition from antiferromagnetism to ferromagnetism offers the possibility to tailor the magnetism and improve the MCE of this magnetic system. In this study, the magnetic properties and MCE of EuTi_0.875Zr_0.125O₃ were systematically investigated by first-principles calculation and experiments. The substitution of Zr induces a significant lattice expansion and alters the electronic interactions, leading to a dominance of ferromagnetism in the compound. Remarkable low-field MCE performance has been achieved attributed to the enhanced ferromagnetism and low saturation field. Under the field change of 0–1 T, the maximum magnetic entropy change (−ΔS_M ^max) and adiabatic temperature change (ΔT_ad ^max) are 17.9 J kg⁻¹ K⁻¹ and 6.1 K, respectively. It is worth noting that the −ΔS_M ^max of EuTi_0.875Zr_0.125O₃ reaches 10.3 J kg⁻¹ K⁻¹ for a field change of 0–0.5 T, making it one of the best magnetocaloric materials ever reported operating in the liquid helium temperature range.