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Spin-orbit-entangled nature of magnetic moments and Kitaev magnetism in layered halides $α$-RuX$_3$ (X = Cl, Br, I)

$α$-RuCl$_3$ has been extensively studied recently because of potential bond-dependent Kitaev magnetic exchange interactions and the resulting quantum spin liquid phase that can be realized therein. It has been known that the covalency between Ru 4$d$- and Cl $p$-orbitals is crucial to induce large Kitaev interactions in this compound, therefore replacing Cl into heavier halogen elements such as Br or I can be a promising way to promote the Kitaev interaction even further. In a timely manner, there have been reports on synthesis of $α$-RuBr$_3$ and $α$-RuI$_3$, which are expected to host the same spin-orbit-entangled orbitals and Kitaev exchange interactions with $α$-RuCl$_3$. Here in this work we investigate electronic structures of $α$-RuCl$_3$, $α$-RuBr$_3$, and $α$-RuI$_3$ in a comparative fashion, focusing on the cooperation of the spin-orbit coupling and on-site Coulomb repulsions to realize the spin-orbit-entangled pseudospin-1/2 at Ru sites. We further estimate magnetic exchange interactions of all three compounds, showing that $α$-RuBr$_3$ can be promising candidates to realize Kitaev spin liquid phases in solid-state systems.