Optical absorption in disordered monolayer molybdenum disulfide

TL;DR

This study investigates how sulfur vacancies and electronic interactions influence the optical absorption of monolayer MoS₂, revealing defect-induced absorption features and potential for solar cell applications.

Contribution

We develop a first-principles-based model combining disorder and electronic interactions to analyze optical properties of monolayer MoS₂, including excitonic effects and defect states.

Findings

Increased sulfur vacancies reduce overall absorption in the band and exciton regions.

Vacancies induce increased sub-bandgap absorption, relevant for defect engineering.

Lifshitz tail behavior accurately described by derived expression.

Abstract

We explore the combined impact of sulfur vacancies and electronic interactions on the optical properties of monolayer MoS$_2$. First, we present a generalized Anderson-Hubbard Hamiltonian that accounts for both randomly distributed sulfur vacancies and the presence of dielectric screening within the material. Second, we parameterize this energy-dependent Hamiltonian from first-principles calculations based on density functional theory and the Green function and screened Coulomb (GW) method. Third, we apply a first-principles-based many-body typical medium method to determine the single-particle electronic structure. Fourth, we solve the Bethe-Salpeter equation to obtain the charge susceptibility $\chi$ with its imaginary part being related to the absorbance $\mathcal{A}$. Our results show that an increased vacancy concentration leads to decreased absorption both in the band continuum and from exciton states within the band gap. We also observe increased absorption below the band gap threshold and present an expression, which describes Lifshitz tails, in excellent qualitative agreement with our numerical calculations. This latter increased absorption in the $1.0$--$2.5$\,eV makes defect engineering of potential interest for solar cell applications.