Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 24, Pages 7910-7915Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b02968
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- University of Bristol
- Alexander von Humboldt Foundation
- Independent Research Fund Denmark
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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.
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