Many-Body Expanded Full Configuration Interaction. I. Weakly Correlated Regime

Abstract

Over the course of the past few decades, the field of computational chemistry has managed to manifest itself as a key complement to more traditional lab-oriented chemistry. This is particularly true in the wake of the recent renaissance of full configuration interaction (FCI)-level methodologies, albeit only if these can prove themselves sufficiently robust and versatile to be routinely applied to a variety of chemical problems of interest. In the present series of works, performance and feature enhancements of one such avenue towards FCI-level results for medium to large one-electron basis sets, the recently introduced many-body expanded full configuration interaction (MBE-FCI) formalism [J. Phys. Chem. Lett., 8, 4633 (2017)], will be presented. Specifically, in this opening part of the series, the capabilities of the MBE-FCI method in producing near-exact ground state energies for weakly correlated molecules of any spin multiplicity will be demonstrated.

38 pages, 7 tables, 3 figures, 1 SI attached as an ancillary file

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• The Ground State Electronic Energy of Benzene
• autoCAS: a program for fully automated multi-configurational calculations
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• Many-Body Expanded Full Configuration Interaction. II. Strongly Correlated Regime
• Machine learning configuration interaction for ab initio potential energy curves
• The performance of CIPSI on the ground state electronic energy of benzene
• Generalized Many-Body Expanded Full Configuration Interaction Theory
• Measuring Electron Correlation. The Impact of Symmetry and Orbital Transformations
• Accurate full configuration interaction correlation energy estimates for five- and six-membered rings
• Molecule-specific Uncertainty Quantification in Quantum Chemical Studies
• Scaling Up Electronic Structure Calculations on Quantum Computers: The Frozen Natural Orbital Based Method of Increments
• Ground- and Excited-State Dipole Moments and Oscillator Strengths of Full Configuration Interaction Quality
• Is Externally Corrected Coupled Cluster Always Better than the Underlying Truncated Configuration Interaction?
• Incremental Treatments of the Full Configuration Interaction Problem
• Towards near-exact solutions of molecular electronic structure: Full coupled-cluster reduction with a second-order perturbative correction
• Ground and Excited State First-Order Properties in Many-Body Expanded Full Configuration Interaction Theory
• Taming the fixed-node error in diffusion Monte Carlo via range separation
• Cluster many-body expansion: a many-body expansion of the electron correlation energy about a cluster mean-field reference
• MBE-CASSCF Approach for the Accurate Treatment of Large Active Spaces
• A hybrid approach to extending selected configuration interaction and full configuration interaction quantum Monte Carlo
• Rationale for the Extrapolation Procedure in Selected Configuration Interaction
• Compactification of Determinant Expansions via Transcorrelation
• Critical Limitations in Quantum-Selected Configuration Interaction Methods
• Addressing Strong Correlation by Approximate Coupled-Pair Methods with Active-Space and Full Treatments of Three-Body Clusters