α-phase ruthenium (III) chloride $\left(\alpha \text{−}{\mathrm{RuCl}}_3\right)$ has attracted significant attention because of its potential for realizing Kitaev quantum spin liquid. In this work, we employ first-principles many-body perturbation theory to study its many-electron interactions and excited-state properties. We find enhanced many-electron interactions that dominate quasiparticle (QP) energies and optical responses in $\alpha \text{−}{\mathrm{RuCl}}_3$. Our calculated QP band gap of the bulk structure is ∼1.75 eV, which agrees well with recent scanning tunneling spectroscopy and angle-resolved photoemission spectroscopy measurements. Furthermore, our calculated first and second primary bright excitons are located at 1.23 and 1.98 eV, respectively. These excitons show good consistency with the main features observed in the optical absorption spectrum. We extend our investigation to monolayer $\alpha \text{−}{\mathrm{RuCl}}_3$, examining the zigzag antiferromagnetic (AFM) and ferromagnetic (FM) phases. In addition to the significant excitonic effect, the optical spectrum of the zigzag AFM phase exhibits anisotropic behavior, while the FM phase demonstrates isotropic characteristics. The different optical response behaviors provide an efficient approach to identify the nearly degenerate energy magnetic states, which can both potentially exist in fabricated samples.

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• Excitons
• Layered crystals
• Bethe-Salpeter equation
• GW method