Chemically tunable quantum magnetism on the anisotropic triangular lattice in rhenium oxyhalides

Masaki Gen (), Daigorou Hirai, Katsuhiro Morita, Kazuhiro Nawa, Satoshi Kogane, Naofumi Matsuyama, Takeshi Yajima, Mitsuaki Kawamura, Kazuhiko Deguchi, Akihiro Koda, Maiko Kofu, Seiko Ohira-Kawamura, Taku J. Sato, Akira Matsuo, Koichi Kindo, Yoshimitsu Kohama and Zenji Hiroi
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Masaki Gen: The University of Tokyo, Institute for Solid State Physics
Daigorou Hirai: The University of Tokyo, Institute for Solid State Physics
Katsuhiro Morita: Tokyo University of Science, Department of Physics, Faculty of Science and Technology
Kazuhiro Nawa: Tohoku University, Institute of Multidisciplinary Research for Advanced Materials (IMRAM)
Satoshi Kogane: The University of Tokyo, Institute for Solid State Physics
Naofumi Matsuyama: The University of Tokyo, Institute for Solid State Physics
Takeshi Yajima: The University of Tokyo, Institute for Solid State Physics
Mitsuaki Kawamura: The University of Tokyo, Institute for Solid State Physics
Kazuhiko Deguchi: Nagoya University, Department of Physics
Akihiro Koda: High Energy Accelerator Research Organization (KEK), Muon Science Laboratory, Institute of Materials Structure Science
Maiko Kofu: Japan Atomic Energy Agency, J-PARC Center
Seiko Ohira-Kawamura: Japan Atomic Energy Agency, J-PARC Center
Taku J. Sato: The University of Tokyo, Institute for Solid State Physics
Akira Matsuo: The University of Tokyo, Institute for Solid State Physics
Koichi Kindo: The University of Tokyo, Institute for Solid State Physics
Yoshimitsu Kohama: The University of Tokyo, Institute for Solid State Physics
Zenji Hiroi: The University of Tokyo, Institute for Solid State Physics

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract The spin-1/2 Heisenberg antiferromagnet on an anisotropic triangular lattice (ATL) is an archetypal spin system hosting exotic quantum magnetism and dimensional crossover. However, the progress in experimental research on this field has been limited due to the scarcity of ideal model materials. Here, we show that rhenium oxyhalides A3ReO5X2, where spin-1/2 Re6+ ions form a layered structure of ATLs, allow for flexible chemical substitution in both cation A2+ (A = Ca, Sr, Ba, Pb) and anion X− (X = Cl, Br) sites, leading to seven synthesizable compounds. By combining magnetic susceptibility and high-field magnetization measurements with theoretical calculations using the orthogonalized finite-temperature Lanczos method, we find that the anisotropy $${J}^{{\prime} }/J$$ J ′ / J ranges from 0.25 to 0.45 depending on the chemical composition. Our findings demonstrate that A3ReO5X2 is an excellent platform for realizing diverse effective spin Hamiltonians that differ in the strength of the anisotropy $${J}^{{\prime} }/J$$ J ′ / J as well as the relevance of perturbation terms such as the Dzyaloshinskii-Moriya interaction and interlayer exchange coupling.

Date: 2025
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DOI: 10.1038/s41467-025-65913-7

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