Chemically inducing room temperature spin-crossover in double layered magnetic refrigerants Pr1.4+Sr1.6-Mn2O7 (0.0 ≤ x ≤ 0.5)

Abstract

The height of total entropy (ST) for a magnetic refrigerant material is essentially concerned with the magnetic and structural transitions. However, the participation of such transitions in layered materials is not well understood. Therefore, the purpose of this work is to investigate the interplay between double layer lattice with their single perovskite counterpart, to achieve optimal magnetocaloric performance. A series of self-doped Pr1.4+xSr1.6-xMn2O7 (0.0 ≤ x ≤ 0.5) Ruddlesden-Popper (R-P) perovskite have been prepared through the solid-state sintering method. With increasing the Pr-stoichiometry, the lattice faults have increased and the double layer lattice dramatically disintegrates into single perovskite structure. Due to the reduction of bilayer R-P phase into single perovskite the spin crossover occurs from weak bilayer (TC = 304 K) interactions towards the strong three-dimensional (TC = 308 K) interactions respectively. This series consistently develops thermomagnetic irreversibility in zero-field cooled (ZFC)-field cooled (FC) magnetization, which is indicative of a spin-glass state. The glassy nature has been ascribed collectively to the lattice strain produced because of dislocations and to an antiferromagnetic phase segregated at the surface. The maximum value of temperature average entropy change (TEC) and adiabatic temperature (ΔTad) has enhanced nearly by 4 folds from 0.53 J kg−1 K−1, 0.59 K (for x = 0.0) up to 1.85 J kg−1 K−1, 10 K (for x = 0.5) at 2.5 T, respectively. Additionally, the room temperature relative cooling power has improved from 26.94 J/kg up to 77.84 J/kg with an applied field of 2.5 T. Our findings in this work suggest that the controlled reduction of double layer lattice into single perovskite and/or existence of both phases simultaneously in bilayer R-P manganites may be very effective in obtaining the desirable characteristics of magnetocaloric effects.