Electronic and magnetic properties of the RuX$_3$ (X=Cl, Br, I) family: Two siblings -- and a cousin? (2203.01626v2)

Abstract: Motivated by recent reports of metallic behavior in the recently synthesized RuI$_3$, in contrast to the Mott-insulating nature of the actively discussed $\alpha$-RuCl$_3$, as well as RuBr$_3$, we present a detailed comparative analysis of the electronic and magnetic properties of this family of trihalides. Using a combination of first-principles calculations and effective-model considerations, we conclude that RuI$_3$, similarly to the other two members, is most probably on the verge of a Mott insulator, but with much smaller magnetic moments and a strong magnetic frustration. We predict the ideal pristine crystal of RuI$_3$ to have a nearly vanishing conventional nearest-neighbor Heisenberg interaction and to be a quantum spin liquid candidate of possibly different kind than the Kitaev spin liquid. In order to understand the apparent contradiction to the reported resistivity $\rho$, we analyze the experimental evidence for all three compounds and propose a scenario for the observed metallicity in existing samples of RuI$_3$. Furthermore, for the Mott insulator RuBr$_3$ we obtain a magnetic Hamiltonian of a similar form to that in the much discussed $\alpha$-RuCl$_3$ and show that this Hamiltonian is in agreement with experimental evidence in RuBr$_3$.