Issue 28, 2024

Cation-placement control in double-perovskite GdBaCo2O6 and its impact on magnetism via spin-state modification

Abstract

Double-perovskite GdBaCo2Ox exhibits remarkable magnetic properties, including half-metallicity, high magnetic anisotropy, and photoinduced magnetic phase transition. While manipulating these properties through cation arrangement is attractive, addressing the thermodynamic stability of the Gd/Ba order necessitates an unconventional synthesis approach. Herein, we report the synthesis of both A-site-ordered and -disordered GdBaCo2O6 films employing a combination of substrate-induced strain and low-temperature topochemical oxidation reactions. Both types of films displayed metallic and ferromagnetic behaviors. Interestingly, the A-site-disordered film exhibited superior magnetization (11.5 μB f.u.−1 at 40 kOe), a higher Curie temperature (TC = 165 K), and lower resistivity compared to the A-site-ordered film (9.5 μB f.u.−1 at 40 kOe; TC = 115 K). Theoretical calculations predicted that the alterations in the magnetic and conductive properties of the A-site-disordered film stem from a change in its Co spin states associated with a change in ion arrangement. This mechanism diverges from conventional double perovskites, where magnetic properties primarily stem from alterations in the combination of nearest-neighbor magnetic elements or lattice parameters without affecting the spin state. Our results highlight the potential of unconventional synthesis strategies in broadening the tunability of functionalities in double-perovskite materials and manipulating spin states through cation-placement control.

Graphical abstract: Cation-placement control in double-perovskite GdBaCo2O6 and its impact on magnetism via spin-state modification

Supplementary files

Article information

Article type
Paper
Submitted
12 Apr 2024
Accepted
20 Jun 2024
First published
21 Jun 2024

J. Mater. Chem. C, 2024,12, 10428-10436

Cation-placement control in double-perovskite GdBaCo2O6 and its impact on magnetism via spin-state modification

T. Katayama, K. Magara, S. Sakai, Y. Zeng, A. Chikamatsu and T. Hasegawa, J. Mater. Chem. C, 2024, 12, 10428 DOI: 10.1039/D4TC01498G

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