Quasiparticle energies and excitonic effects of {\alpha}-RuCl3

TL;DR

This study uses first-principles calculations to analyze quasiparticle energies and excitonic effects in {eta}-RuCl3, revealing key electronic and optical properties relevant for quantum spin liquid research.

Contribution

It provides the first comprehensive theoretical analysis of quasiparticle energies and excitonic effects in {eta}-RuCl3, including magnetic phase-dependent optical responses.

Findings

Quasiparticle band gap of about 1.75 eV in bulk {eta}-RuCl3.

Identification of primary bright excitons at 1.23 eV and 1.98 eV.

Distinct optical anisotropy in zigzag AFM phase compared to FM phase.

Abstract

{\alpha}-phase Ruthenium (III) chloride ({\alpha}-RuCl3) 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 energies and optical responses in {\alpha}-RuCl3. Our calculated quasiparticle band gap of bulk structure is about 1.75 eV that 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 eV 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}-RuCl3, examining the zigzag antiferromagnetic (AFM) and ferromagnetic (FM) phases. In addition to significant excitonic effects, 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 energy nearly degenerate magnetic states, which can both potentially exist in fabricated samples.