Electron correlation in solids via density embedding theory

TL;DR

This paper extends density embedding theory to infinite solids, enabling accurate electronic structure calculations with reduced computational cost by using Wannier functions and coupled cluster methods.

Contribution

It introduces a formalism for applying density embedding theory to infinite systems, including defining impurity Hamiltonians and addressing state disentanglement.

Findings

Results comparable to full coupled cluster calculations for infinite systems.

Effective in 1D, 2D, and 3D cases using a single unit cell.

Does not require localization of unoccupied bands.

Abstract

Density matrix embedding theory (Phys. Rev. Lett. 109, 186404 (2012)) and density embedding theory ((Phys. Rev. B 89, 035140 (2014)) have recently been introduced for model lattice Hamiltonians and molecular systems. In the present work, the formalism is extended to the ab initio description of infinite systems. An appropriate definition of the impurity Hamiltonian for such systems is presented and demonstrated in cases of 1, 2 and 3 dimensions, using coupled cluster theory as the impurity solver. Additionally, we discuss the challenges related to disentanglement of fragment and bath states. The current approach yields results comparable to coupled cluster calculations of infinite systems even when using a single unit cell as the fragment. The theory is formulated in the basis of Wannier functions but it does not require separate localization of unoccupied bands. The embedding scheme presented here is a promising way of employing highly accurate electronic structure methods for extended systems at a fraction of their original computational cost.