6533b7d4fe1ef96bd1261f17
RESEARCH PRODUCT
Generalized Many-Body Expanded Full Configuration Interaction Theory
Jürgen GaussJanus J. Eriksensubject
Chemical Physics (physics.chem-ph)010304 chemical physicsBasis (linear algebra)Computer scienceFOS: Physical sciences010402 general chemistrySpace (mathematics)01 natural sciencesFull configuration interactionMany body0104 chemical sciencesTheoretical physicsAtomic orbitalPhysics - Chemical Physics0103 physical sciencesGeneral Materials ScienceAstrophysics::Earth and Planetary AstrophysicsPhysical and Theoretical Chemistrydescription
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 a 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.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2019-11-28 |