2–5 Jun 2025
Europe/Paris timezone

Bond-dependent interactions and ill-ordered state in the honeycomb cobaltate BaCo2(AsO4)2

2 Jun 2025, 16:00
15m

Speaker

Armand Devillez (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France)

Description

Following the proposed materialization of Kitaev-bond-dependent spin liquid physics in honeycomb lattices of heavy transition metals with 4d or 5d electrons [1], it has been proposed that this can be extended to 3d transition metals, in particular Co2+ [2]. A first step in validating the prospect of finding a quantum spin liquid is to demonstrate the presence of these anisotropic bond-dependent interactions in such materials. These could promote new types of behavior or provide insight into certain materials not elucidated to date. This is the case of BaCo2(AsO4)2, a honeycomb cobaltate whose ground state and Hamiltonian have been debated for decades [3]. We have investigated the magnetic properties of a BaCo2(AsO4)2 single-crystal through neutron diffraction and inelastic scattering, as well as by very-low temperature magnetization and AC susceptibility measurements. The latter measurements, which reveal slow dynamics and non-equilibrium responses, are consistent with an original ill-ordered magnetic compound with intrinsic defects as proposed previously [4]: collinear zig-zag ferromagnetic chains in a up-up-down-down arrangement interspersed with additional chains to agree with the propagation vector of 0.27 imposed by competing interactions. To interpret these results, we propose an exchange model with bond-dependent anisotropic interactions on the first neighbors and Heisenberg interactions up to the fourth neighbors. Monte Carlo calculations show that our model successfully reproduces key experimental observations, namely spin-wave dispersions (figure), magnetization curves with a 1/3 magnetization plateau, and the faulty collinear spin configuration, leading to a coherent picture that had not been achieved to date [5]. This highlights the potential of including these new ingredients (anisotropic Kitaev and off-diagonal interactions) in understanding long-standing puzzling behaviors and discovering exotic physics.

References:
[1] A. Kitaev, Ann. Phys. 321, 2 (2006) ; G. Jackeli and G. Khaliullin, Phys. Rev. Lett. 102, (2009).
[2] H. Liu and G. Khaliullin, Phys. Rev. B 97, 014407 (2018) ; R. Sano, Y. Kato, and Y. Motome, Physical Review B 97, 014408 (2018).
[3] L.-P. Regnault, J. Rossat-Mignod, and J. Y. Henry, J. Phys. Soc. Jpn. 52, 1 (1983) ; R. Zhong, T. Gao, N. P. Ong, and R. J. Cava, Science advances 6, 1 (2020) ; P. A. Maksimov, A. V. Ushakov, Z. V. Pchelkina, Y. Li, S. M. Winter, and S. V. Streltsov, Physical Review B 106, 165131 (2022) ; T. Halloran, F. Desrochers, E. Z. Zhang, T. Chen, L. E. Chern, Z. Xu, B. Winn, M. Graves-Brook, M. B. Stone, A. I. Kolesnikov, Y. Qiu, R. Zhong, R. Cava, Y. B. Kim, and C. Broholm, PNAS 120, e2215509119 (2023).
[4] L.-P. Regnault, C. Boullier, and J. E. Lorenzo, Heliyon 4, e00507 (2018).
[5] A. Devillez, J. Robert, E. Lhotel, R. Ballou, F. Denis-Romero, Q. Faure, E. Ressouche, H. Jacobsen, J. Lass, D. Mazzone, U. Bengaard Hansen, M. Enderle, S. Raymond, S. De Brion, V. Simonet, and M. Songvilay, in preparation

Primary author

Armand Devillez (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France)

Co-authors

Daniel Mazzone (Laboratory for Neutron Scattering and Imaging (LNS), Paul Scherrer Institut (PSI), 5232 Villigen PSI, Switzerland) Elsa Lhotel (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France) Eric Ressouche (Université Grenoble Alpes, CEA, IRIG, MEM, MDN, 38042 Grenoble, France) Henrick Jacobsen (Laboratory for Neutron Scattering and Imaging (LNS), Paul Scherrer Institut (PSI), 5232 Villigen PSI, Switzerland, Nanoscience Center, Niels Bohr Institute, University of Copenhagen, 2100 Copenhagen, Denmark) Jakob Lass (Laboratory for Neutron Scattering and Imaging (LNS), Paul Scherrer Institut (PSI), 5232 Villigen PSI, Switzerland) Julien Robert (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France) Manila Songvilay (Institut Néel, Grenoble) Rafik Ballou (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France) Sophie De Brion (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France) Virginie Simonet (Université Grenoble Alpes, CNRS, Institut Néel, 38042 Grenoble, France)

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