Electron Correlation in 2D Periodic Systems from Periodic Bootstrap Embedding

Given the growing significance of 2D materials in various optoelectronic applications, it is imperative to have simulation tools that can accurately and efficiently describe electron correlation effects in these systems. Here, we show that the recently developed bootstrap embedding (BE) accurately predicts electron correlation energies and structural properties for 2D systems. Without explicit dependence on the reciprocal space sum (k-points) in the correlation calculation, our proof-of-concept calculations shows that BE can typically recover ∼99.5% of the total minimal basis electron correlation energy in 2D semimetal, insulator, and semiconductors. We demonstrate that BE can predict lattice constants and bulk moduli for 2D systems with high precision. Furthermore, we highlight the capability of BE to treat electron correlation in twisted bilayer graphene superlattices with large unit cells containing hundreds of carbon atoms. We find that as the twist angle decreases toward the magic angle, the correlation energy initially decreases in magnitude, followed by a subsequent increase. We conclude that BE is a promising electronic structure method for future applications to 2D materials.