Pressure-dependent magnetism of the Kitaev candidate Li${}_2$RhO${}_3$

Abstract

We use magnetization measurements under pressure along with \textit{ab initio} and cluster many-body calculations to investigate magnetism of the Kitaev candidate Li${}_2$RhO${}_3$. Hydrostatic compression leads to a decrease in the magnitude of the nearest-neighbor ferromagnetic Kitaev coupling $K_1$ and the corresponding increase in the off-diagonal anisotropy ${\Gamma }_1$, whereas the experimental Curie-Weiss temperature changes from negative to positive with the slope of +40~K/GPa. On the other hand, spin freezing persists up to at least 3.46~GPa with the almost constant freezing temperature of 5~K that does not follow the large changes in the exchange couplings and indicates the likely extrinsic origin of spin freezing. Magnetic frustration in Li${}_2$RhO${}_3$ is mainly related to the interplay between ferromagnetic $K_1$ and antiferromagnetic ${\Gamma }_1$, along with the weakness of the third-neighbor coupling $J_3$ that would otherwise stabilize zigzag order. The small $J_3$ distinguishes Li${}_2$RhO${}_3$ from other Kitaev candidates.

Main text: 10 pages, 6 figures. Supplemental material: 4 pages, 3 figures

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