Year: 2018
Type: article
Abstract: We explore the combined impact of sulfur vacancies and electronic interactions on the optical properties of monolayer ${\mathrm{MoS}}_{2}$. 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 parametrize this energy-dependent Hamiltonian from first-principles calculations based on density functional theory and the Green's 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 $\ensuremath{\chi}$ 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 $1.0--2.5\phantom{\rule{0.28em}{0ex}}\mathrm{eV}$ range makes defect engineering of potential interest for solar cell applications.
Authors: C. E. Ekuma, D. Gunlycke
Institution: United States Naval Research Laboratory
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W2806284288