Generalized Many-Body Expanded Full Configuration Interaction Theory

Janus J. Eriksen*, Jürgen Gauss

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)

2 Citations (Scopus)

Abstract

Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body expanded full configuration interaction (MBE-FCI) method to allow for electron-rich model and molecular systems dominated by both weak and strong correlation to be addressed. By employing minimal or even empty reference spaces, we show through calculations on the one-dimensional Hubbard model with up to 46 lattice sites, the chromium dimer, and the benzene molecule how near-exact results may be obtained in an entirely unbiased manner for chemical and physical problems of not only academic but also applied chemical interest. Given the massive parallelism and overall accuracy of the resulting method, we argue that generalized MBE-FCI theory possesses an immense potential to yield near-exact correlation energies for molecular systems of unprecedented size, composition, and complexity in the years to come.

Original languageEnglish
Pages (from-to)7910-7915
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume10
Issue number24
Early online date27 Nov 2019
DOIs
Publication statusPublished - 19 Dec 2019

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