Glassy Magnetic Transitions and Accurate Estimation of Magnetocaloric Effect in Ni–Mn Heusler Alloys

In this work, the structural and magnetic transitions of Heusler alloy Ni₅₀Mn₃₄In₁₄Ga₂ have been carefully studied through measurements of heat flow and magnetization under DC and AC magnetic fields. This alloy undergoes the transition sequence of spin-glassy martensite (SPM) → ferromagnetic austenite (FA) → paramagnetic austenite at ∼225 and ∼305 K, respectively, during heating. Splitting of zero-field-cooling (ZFC)/field-cooling (FC) curves in martensite is caused by the slowdown dynamics of spin glass as evidenced by frequency dispersion and aging effects. The development of a spin-glass state is believed to be the result of strain relaxation and interaction of ferroelastic twin walls in the martensite. The magnetocaloric effect (MCE) at the SPM-FA transition was then measured using indirect, quasi-direct, and direct methods. The MCE magnitudes are controlled by the entropy changes associated with the first-order martensite transition and magnetic ordering of austenite under the magnetic field. The existence of a spin-glass state in martensite can also improve the reversibility of the magnetostructural transitions, which is beneficial for the improvement of the reversibility of associated MCE. These results provide an in-depth understanding of the transitions and magnetic properties of the Ni-Mn Heusler alloys and suggest that the MCE at the first-order magnetostructural transitions estimated solely using indirect methods may need some revision.