Spin-orbit driven = magnetism in a triangular-lattice monolayer cobaltate
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 electronic configuration as promising hosts for spin-orbit entangled 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 cobaltates as a compelling platform for frustrated magnetism. Here we investigate a representative triangular-lattice monolayer cobaltate , where first-principles density functional theory (DFT) calculations reveal a dominant nearest-neighbor hopping channel that enhances the ferromagnetic Kitaev-type exchange interactions. In contrast, the nearest-neighbor Heisenberg term is highly sensitive to a direct 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 () and third () nearest neighbor Heisenberg exchange dependent magnetic phase diagram in the physically relevant regime and identify multiple competing ground states, including ferromagnetic, stripy, incommensurate, and antiferromagnetic orders. The Luttinger-Tisza analysis further predicts a 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 systems, our results on monolayer establish 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.