Geometrically frustrated Gd2Ti2O7 oxide: A comprehensive exploration of structural, magnetic, and magnetocaloric properties for cryogenic magnetic cooling applications

Abstract

The magnetocaloric effect (MCE) has been extensively studied in various magnetic solids, aiming to both facilitate practical applications in magnetic cooling and deepen our understanding these materials’ intrinsic properties. This study presents a systematic investigation of Gd2Ti2O7 oxide, characterized by a geometrically frustrated magnetic structure, focusing on its structural and magnetic characteristics through experimental analysis and theoretical calculations. Emphasis is placed on its magnetic phase transition (MPT) and magnetocaloric properties, scrutinizing temperatures as low as 0.4 K and magnetic fields up to 16 T. The results reveal that Gd2Ti2O7 oxide possesses a crystalline cubic pyrochlore-type structure with an antiferromagnetic (AFM) semiconductor ground state. The material undergoes a first-order MPT in low field and low-temperature regimes, transitioning to a second-order MPT above 2 K up to 16 T. Evaluation of magnetocaloric parameters, including maximum magnetic entropy change, temperature-averaged entropy change, relative cooling power, and refrigerant capacity, indicates moderate values under low magnetic field changes, while significantly large values are achievable under high magnetic field changes. This finding suggests that potential cryogenic magnetocaloric materials (MCMs) with optimal performance should exhibit low MPT temperatures induced by magnetic frustration and possess a ground state with a sufficiently large magnetic moment induced by low magnetic fields, thus avoiding excessively strong AFM coupling. This study lays the groundwork for future cryogenic MCM design and provides valuable insights into the intrinsic properties of geometrically frustrated magnetic materials.