Magnetic and Magnetocaloric Properties of the A2LnSbO6 Lanthanide Oxides on the Frustrated fcc Lattice

Elise Anne C. Koskelo; Nicola D. Kelly; Liam A.V. Nagle-Cocco; Joshua D. Bocarsly; Paromita Mukherjee; Cheng Liu; Qiang Zhang; Siân E. Dutton

doi:10.1021/acs.inorgchem.3c01137

Magnetic and Magnetocaloric Properties of the A₂LnSbO₆ Lanthanide Oxides on the Frustrated fcc Lattice

Elise Anne C. Koskelo, Nicola D. Kelly, Liam A.V. Nagle-Cocco, Joshua D. Bocarsly, Paromita Mukherjee, Cheng Liu, Qiang Zhang, Siân E. Dutton

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Abstract

Frustrated lanthanide oxides are promising candidates for cryogen-free magnetic refrigeration due to their suppressed ordering temperatures and high magnetic moments. While much attention has been paid to the garnet and pyrochlore lattices, the magnetocaloric effect in frustrated face-centered cubic (fcc) lattices remains relatively unexplored. We previously showed that the frustrated fcc double perovskite Ba₂GdSbO₆ is a top-performing magnetocaloric material (per mol Gd) because of its small nearest-neighbor interaction between spins. Here we investigate different tuning parameters to maximize the magnetocaloric effect in the family of fcc lanthanide oxides, A₂LnSbO₆ (A = {Ba²⁺, Sr²⁺} and Ln = {Nd³⁺, Tb³⁺, Gd³⁺, Ho³⁺, Dy³⁺, Er³⁺}), including chemical pressure via the A site cation and the magnetic ground state via the lanthanide ion. Bulk magnetic measurements indicate a possible trend between magnetic short-range fluctuations and the field-temperature phase space of the magnetocaloric effect, determined by whether an ion is a Kramers or a non-Kramers ion. We report for the first time on the synthesis and magnetic characterization of the Ca₂LnSbO₆ series with tunable site disorder that can be used to control the deviations from Curie-Weiss behavior. Taken together, these results suggest fcc lanthanide oxides as tunable systems for magnetocaloric design.

Original language	English
Pages (from-to)	10317-10328
Number of pages	12
Journal	Inorganic Chemistry
Volume	62
Issue number	26
DOIs	https://doi.org/10.1021/acs.inorgchem.3c01137
State	Published - Jul 3 2023

Funding

This work was supported through the EP/T028580/1 EPSRC Grant and the Winton Programme for the Physics of Sustainability. E.C.K. gratefully acknowledges the support of a Churchill Scholarship from the Winston Churchill Foundation of the United States. Magnetic measurements were made on the EPSRC Advanced Characterization Suite EP/M0005/24/1. L.N.C. and N.D.K. acknowledge Ph.D. funding from the EPSRC under scholarship EP/R513180/1. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. We thank Venkat Daramalla and Clare Grey for insightful discussions about this work.

Funders	Funder number
Office of Science
Oak Ridge National Laboratory
Winston Churchill Foundation of the United States	EP/R513180/1
Engineering and Physical Sciences Research Council

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10.1021/acs.inorgchem.3c01137

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title = "Magnetic and Magnetocaloric Properties of the A2LnSbO6 Lanthanide Oxides on the Frustrated fcc Lattice",

abstract = "Frustrated lanthanide oxides are promising candidates for cryogen-free magnetic refrigeration due to their suppressed ordering temperatures and high magnetic moments. While much attention has been paid to the garnet and pyrochlore lattices, the magnetocaloric effect in frustrated face-centered cubic (fcc) lattices remains relatively unexplored. We previously showed that the frustrated fcc double perovskite Ba2GdSbO6 is a top-performing magnetocaloric material (per mol Gd) because of its small nearest-neighbor interaction between spins. Here we investigate different tuning parameters to maximize the magnetocaloric effect in the family of fcc lanthanide oxides, A2LnSbO6 (A = {Ba2+, Sr2+} and Ln = {Nd3+, Tb3+, Gd3+, Ho3+, Dy3+, Er3+}), including chemical pressure via the A site cation and the magnetic ground state via the lanthanide ion. Bulk magnetic measurements indicate a possible trend between magnetic short-range fluctuations and the field-temperature phase space of the magnetocaloric effect, determined by whether an ion is a Kramers or a non-Kramers ion. We report for the first time on the synthesis and magnetic characterization of the Ca2LnSbO6 series with tunable site disorder that can be used to control the deviations from Curie-Weiss behavior. Taken together, these results suggest fcc lanthanide oxides as tunable systems for magnetocaloric design.",

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AU - Bocarsly, Joshua D.

AU - Mukherjee, Paromita

AU - Liu, Cheng

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AB - Frustrated lanthanide oxides are promising candidates for cryogen-free magnetic refrigeration due to their suppressed ordering temperatures and high magnetic moments. While much attention has been paid to the garnet and pyrochlore lattices, the magnetocaloric effect in frustrated face-centered cubic (fcc) lattices remains relatively unexplored. We previously showed that the frustrated fcc double perovskite Ba2GdSbO6 is a top-performing magnetocaloric material (per mol Gd) because of its small nearest-neighbor interaction between spins. Here we investigate different tuning parameters to maximize the magnetocaloric effect in the family of fcc lanthanide oxides, A2LnSbO6 (A = {Ba2+, Sr2+} and Ln = {Nd3+, Tb3+, Gd3+, Ho3+, Dy3+, Er3+}), including chemical pressure via the A site cation and the magnetic ground state via the lanthanide ion. Bulk magnetic measurements indicate a possible trend between magnetic short-range fluctuations and the field-temperature phase space of the magnetocaloric effect, determined by whether an ion is a Kramers or a non-Kramers ion. We report for the first time on the synthesis and magnetic characterization of the Ca2LnSbO6 series with tunable site disorder that can be used to control the deviations from Curie-Weiss behavior. Taken together, these results suggest fcc lanthanide oxides as tunable systems for magnetocaloric design.

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Magnetic and Magnetocaloric Properties of the A₂LnSbO₆ Lanthanide Oxides on the Frustrated fcc Lattice

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