Applying the Coupled-Cluster Ansatz to Solids and Surfaces in the Thermodynamic Limit

Abstract

Modern electronic structure theories can predict and simulate a wealth of phenomena in surface science and solid-state physics. In order to allow for a direct comparison with experiment, such ab initio predictions have to be made in the thermodynamic limit, substantially increasing the computational cost of many-electron wave-function theories. Here, we present a method that achieves thermodynamic limit results for solids and surfaces using the "gold standard" coupled cluster ansatz of quantum chemistry with unprecedented efficiency. We study the energy difference between carbon diamond and graphite crystals, adsorption energies of water on h-BN, as well as the cohesive energy of the Ne solid, demonstrating the increased efficiency and accuracy of coupled cluster theory for solids and surfaces.

4 figures

References in corpus (2)

• The Finite Size Error in Many-body Simulations with long-Ranged Interactions
• Finite-size correction in many-body electronic structure calculations

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• An optimized twist angle to find the twist-averaged correlation energy applied to the uniform electron gas
• First principles correction scheme for linear-response time-dependent density functional theory calculations of core electronic states
• Periodic Coupled-Cluster Green's Function for Photoemission Spectra of Realistic Solids
• Accurate thermochemistry of covalent and ionic solids from spin-component-scaled MP2
• Approaching the basis-set limit of the dRPA correlation energy with explicitly correlated and Projector Augmented-wave methods
• Accelerating convergence to the thermodynamic limit with twist angle selection applied to methods beyond many-body perturbation theory
• Structural and electronic properties of solid molecular hydrogen from many-electron theories