Electron correlation in solids via density embedding theory
- Department of Chemistry, Rice University, Houston, Texas 77005 (United States)
Density matrix embedding theory [G. Knizia and G. K.-L. Chan, Phys. Rev. Lett. 109, 186404 (2012)] and density embedding theory [I. W. Bulik, G. E. Scuseria, and J. Dukelsky, 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.
- OSTI ID:
- 22419987
- Journal Information:
- Journal of Chemical Physics, Vol. 141, Issue 5; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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