Correlating Crystallography, Magnetism, and Electronic Structure Across Anhysteretic First-Order Phase Transition in Pr2In

Abstract

Temperature-dependent powder X-ray diffraction and magnetization measurements of Pr2In conclusively prove that the unusual anhysteretic first-order paramagnetic-ferromagnetic phase transition in the compound is related to concurrent changes in both the magnetic and crystallographic lattices. At the same time, the hexagonal Ni2In-type structure is stable at least between 6 and 298 K, including at T C = ∼57 K. From the density functional theory calculations, the electronic structure of the compound is extraordinarily sensitive to minor changes in lattice parameters that occur across the phase transition, revealing the origin of strong magnetoelastic coupling. In the vicinity of T C, the maximum entropy change, ΔS Max = −16 J Kg−1 K−1 induced by a moderate magnetic field change of 20 kOe (ΔS Max = −20 J Kg−1 K−1 for 50 kOe magnetic field change) is comparable to other known potentially functional materials demonstrating large cryogenic magnetocaloric effect.