Coordinate descent full configuration interaction

Abstract

We develop an efficient algorithm, coordinate descent FCI (CDFCI), for the electronic structure ground state calculation in the configuration interaction framework. CDFCI solves an unconstrained non-convex optimization problem, which is a reformulation of the full configuration interaction eigenvalue problem, via an adaptive coordinate descent method with a deterministic compression strategy. CDFCI captures and updates appreciative determinants with different frequencies proportional to their importance. We show that CDFCI produces accurate variational energy for both static and dynamic correlation by benchmarking the binding curve of nitrogen dimer in the cc-pVDZ basis with $10^{-3}$ mHa accuracy. We also demonstrate the efficiency and accuracy of CDFCI for strongly correlated chromium dimer in the Ahlrichs VDZ basis and produces state-of-the-art variational energy.

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Cited by in corpus (23)

• The Ground State Electronic Energy of Benzene
• NECI: N-Electron Configuration Interaction with emphasis on state-of-the-art stochastic methods
• The Shape of Full Configuration Interaction to Come
• Machine learning configuration interaction for ab initio potential energy curves
• Generalized Many-Body Expanded Full Configuration Interaction Theory
• Efficient and Stochastic Multireference Perturbation Theory for Large Active Spaces within a Full Configuration Interaction Quantum Monte Carlo Framework
• SOiCI and iCISO: Combining iterative configuration interaction with spin-orbit coupling in two ways
• Dual-Cone Variational Calculation of the 2-Electron Reduced Density Matrix
• Exact Two-body Expansion of the Many-particle Wave Function
• Ground and Excited State First-Order Properties in Many-Body Expanded Full Configuration Interaction Theory
• Cluster many-body expansion: a many-body expansion of the electron correlation energy about a cluster mean-field reference
• Optimal Orbital Selection for Full Configuration Interaction (OptOrbFCI): Pursuing the Basis Set Limit under a Budget
• A greedy algorithm for computing eigenvalues of a symmetric matrix
• Hamiltonian models of lattice fermions solvable by the meron-cluster algorithm
• A Power Series Approximation in Symmetry Projected Coupled Cluster Theory
• Alternating Descent Method for Gauge Cooling of Complex Langevin Simulations
• Beyond Walkers in Stochastic Quantum Chemistry: Reducing Error using Fast Randomized Iteration
• Triangularized Orthogonalization-free Method for Solving Extreme Eigenvalue Problems
• Solving the k-sparse Eigenvalue Problem with Reinforcement Learning
• Further Development of iCIPT2 for Strongly Correlated Electrons
• Approaching the Full Configuration Interaction Ground State from an Arbitrary Wavefunction with Gradient Descent and Quasi-Newton Algorithms
• Improved Fast Randomized Iteration Approach to Full Configuration Interaction
• A Finite Element Configuration Interaction Method for Wigner Localization