Spin-Orbit-Entangled Nature of Magnetic Moments and Kitaev Magnetism in Layered Halides

$\alpha$-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 $\alpha$-RuBr$_3$ and $\alpha$-RuI$_3$, which are expected to host the same spin-orbit-entangled orbitals and Kitaev exchange interactions with $\alpha$-RuCl$_3$. Here in this work we investigate electronic structures of $\alpha$-RuCl$_3$, $\alpha$-RuBr$_3$, and $\alpha$-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 $\alpha$-RuBr$_3$ can be promising candidates to realize Kitaev spin liquid phases in solid-state systems.