Impact of mixed anion ordered state on the magnetic ground states of S=1/2 square-lattice quantum spin antiferromagnets, Sr2NiO3Cl and Sr2NiO3F

Tsujimoto, Y; Sugiyama, J; Ochi, M; Kuroki, K; Manuel, P; Khalyavin, DD; Umegaki, I; Månsson, M; Andreica, D; Hara, S; Sakurai, T; Okubo, S; Ohta, H; Boothroyd, AT; Yamaura, K

Journal article

Impact of mixed anion ordered state on the magnetic ground states of S=1/2 square-lattice quantum spin antiferromagnets, Sr2NiO3Cl and Sr2NiO3F

Abstract:: The magnetic properties of the S=1/2 two-dimensional square-lattice antiferromagnets Sr2NiO3X (X=Cl, F) with the trivalent nickel ions in a low-spin state were studied by magnetic susceptibility, heat capacity, neutron powder diffraction, high-field electron spin resonance (ESR), muon spin rotation and relaxation (μ+SR) measurements, and density functional theory (DFT) calculations. Both oxyhalides are isostructural to an ideal quantum square-lattice antiferromagnet Sr2CuO2Cl2, but the chlorine/fluorine anion exclusively occupies an apical site in an ordered/disordered manner with an oxygen anion, resulting in the formation of highly distorted NiO5X octahedra with an off-center nickel ion. Magnetic susceptibility measurements revealed a remarkable difference between these two compounds: the magnetic susceptibility of Sr2NiO3Cl exhibited a broad maximum at approximately 35 K, which is typical of low-dimensional antiferromagnetic behavior. In contrast, the magnetic susceptibility of Sr2NiO3F exhibited spin-glass-like behavior below 12 K. No anomaly associated with long-range magnetic ordering was observed in the heat capacity, ESR, and neutron powder diffraction experiments. However, μ+SR measurements revealed the emergence of a static magnetic ordered state below TN=28K in Sr2NiO3Cl and a short-range magnetic state below TN=18K in Sr2NiO3F. The DFT calculations suggested that the unpaired electron occupied a d3z2-r2 orbital, and ferromagnetic couplings between the nearest-neighbor nickel spins were energetically favored. The mechanism of ferromagnetic superexchange interactions and the reason for the difference between the magnetic ground states in these nickel oxyhalides are discussed.

Publication status:: Published

Peer review status:: Peer reviewed

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APA Style

Tsujimoto, Y., Sugiyama, J., Ochi, M., Kuroki, K., Manuel, P., Khalyavin, D. D., Umegaki, I., Månsson, M., Andreica, D., Hara, S., Sakurai, T., Okubo, S., Ohta, H., Boothroyd, A. T., & Yamaura, K. (2022). Impact of mixed anion ordered state on the magnetic ground states of S=1/2 square-lattice quantum spin antiferromagnets, Sr2NiO3Cl and Sr2NiO3F. Physical Review Materials, 6(11).

MLA Style

Tsujimoto, Y., et al. “Impact of Mixed Anion Ordered State on the Magnetic Ground States of S=1/2 Square-Lattice Quantum Spin Antiferromagnets, Sr2NiO3Cl and Sr2NiO3F.” Physical Review Materials, vol. 6, no. 11, American Physical Society, 2022.

Chicago Style

Tsujimoto, Y, J Sugiyama, M Ochi, K Kuroki, P Manuel, DD Khalyavin, I Umegaki, et al. 2022. “Impact of Mixed Anion Ordered State on the Magnetic Ground States of S=1/2 Square-Lattice Quantum Spin Antiferromagnets, Sr2NiO3Cl and Sr2NiO3F.” Physical Review Materials 6 (11).
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