First principles coupled cluster theory of the electronic spectrum of the transition metal dichalcogenides

Abstract

The electronic properties of two-dimensional transition metal dichalcogenides (2D TMDs) have attracted much attention during the last decade. We show how a diagrammatic ab initio coupled cluster singles and doubles (CCSD) treatment paired with a careful thermodynamic limit extrapolation in two dimensions can be used to obtain converged bandgaps for monolayer materials in the MoS2 family. We find general agreement between CCSD and previously reported GW simulations in terms of the band structure, but predict slightly higher band gap values and effective hole masses compared to previous reports. We also investigate the ability of CCSD to describe trion states, finding reasonable qualitative structure, but poor excitation energies due to the lack of screening of three-particle excitations in the effective Hamiltonian. Our study provides an independent high-level benchmark of the role of many-body effects in 2D TMDs and showcases the potential strengths and weaknesses of diagrammatic coupled cluster approaches for realistic materials.

arXiv comment5 pages, 4 figures

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• A periodic equation-of-motion coupled-cluster implementation applied to $F$-centers in alkaline earth oxides
• Critical assessment of $G_0{W}_0$ calculations for 2D materials: the example of monolayer MoS${}_2$
• Unitary coupled-cluster based self-consistent polarization propagator theory: a quadratic unitary coupled-cluster singles and doubles scheme
• Dynamical correlation energy of metals in large basis sets from downfolding and composite approaches
• Toward improved property prediction of 2D materials using many-body quantum Monte Carlo methods
• Equation of state of atomic solid hydrogen by stochastic many-body wave function methods
• Excitations of Quantum Many-Body Systems via Purified Ensembles: A Unitary-Coupled-Cluster-based Approach
• Resolving Finite-Size Errors in EOM-CCSD Band Gaps of Solids with Interacting-Bath Dynamical Embedding Theory