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    Spin-orbit driven Jeff = 12 magnetism in a d7 triangular-lattice monolayer cobaltate

    Ritwik Das*, Soumen Basak, Mohammad Rezwan Habib, and Indra Dasgupta†

    • *Contact author: intrd@iacs.res.in
    • †Contact author: sspid@iacs.res.in

    Phys. Rev. B 113, 205137 – Published 20 May, 2026

    DOI: https://doi.org/10.1103/x8r8-k65m

    Abstract

    Recent theoretical and experimental advances have identified cobaltates with a high-spin d7 electronic configuration as promising hosts for spin-orbit entangled Jeff=1/2 magnetism that can support bond-dependent exchange interactions. In two-dimensional triangular lattices, the coexistence of such exchange frustration along with usual geometric frustration gives rise to a rich landscape of competing magnetic phases, establishing monolayer triangular d7 cobaltates as a compelling platform for frustrated magnetism. Here we investigate a representative triangular-lattice monolayer cobaltate CoBr2, where first-principles density functional theory (DFT) calculations reveal a dominant nearest-neighbor t2g–eg hopping channel that enhances the ferromagnetic Kitaev-type exchange interactions. In contrast, the nearest-neighbor Heisenberg term is highly sensitive to a direct t2g–t2g hopping path and electronic correlations. The magnetic exchange parameters are evaluated using the hopping amplitudes obtained from DFT calculations within an exact diagonalization framework. We construct the first (J1) and third (J3) nearest neighbor Heisenberg exchange dependent J1–J3 magnetic phase diagram in the physically relevant regime and identify multiple competing ground states, including ferromagnetic, stripy, incommensurate, and 120∘ antiferromagnetic orders. The Luttinger-Tisza analysis further predicts a Z2 vortex crystal phase, while exact diagonalization reveals a bond-nematic phase promoted by quantum fluctuations. Going beyond the conventional bond-independent XXZ picture typically applied to Co2+ systems, our results on monolayer CoBr2 establish d7 cobalt dihalides as a promising platform to explore the interplay of long-range Heisenberg and bond-dependent exchange interactions that can stabilize diverse magnetic ground states on a triangular lattice.

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