Gaussian-based coupled-cluster theory for the ground state and band structure of solids

TL;DR

This paper applies Gaussian-based coupled-cluster methods to accurately compute ground-state properties and band structures of covalent semiconductors like diamond and silicon, demonstrating high-precision results for solids.

Contribution

It introduces a Gaussian-based coupled-cluster approach for solids, enabling detailed ground and excited state calculations with high accuracy.

Findings

Accurate lattice constants, bulk modulus, and cohesive energies obtained.

Quasiparticle band structures and gaps computed with extensive Brillouin zone sampling.

Method demonstrates feasibility for large-scale solid-state quantum chemistry calculations.

Abstract

We present the results of Gaussian-based ground-state and excited-state equation-of-motion coupled-cluster theory with single and double excitations for three-dimensional solids. We focus on diamond and silicon, which are paradigmatic covalent semiconductors. In addition to ground-state properties (the lattice constant, bulk modulus, and cohesive energy), we compute the quasiparticle band structure and band gap. We sample the Brillouin zone with up to 64 k-points using norm-conserving pseudopotentials and polarized double- and triple-zeta basis sets, leading to canonical coupled-cluster calculations with as many as 256 electrons in 2,176 orbitals.