OpenOrbitalOptimizer -- a reusable open source library for self-consistent field calculations

Abstract

According to the modern paradigms of software engineering, standard tasks are best accomplished by reusable open source libraries. We describe OpenOrbitalOptimizer: a reusable open source C++ library for the iterative solution of coupled self-consistent field (SCF) equations ${\mathbf{F}}_p^{\sigma }(\{{\mathbf{C}}_p^{\sigma }\}){\mathbf{C}}_p^{\sigma }={\mathbf{C}}_p^{\sigma }{\mathbf{E}}_p^{\sigma }$ for an arbitrary number of particle types $p$ and symmetries. Although OpenOrbitalOptimizer is a new project, it already implements standard algorithms for solving SCF equations: Pulay's direct inversion in the iterative subspace (DIIS), energy DIIS (EDIIS), augmented DIIS (ADIIS), and the optimal damping algorithm (ODA). The library was designed as an easy way to introduce the state-of-the-art convergence accelerators in a number of legacy programs. It is easy to interface with various programs, as it only requires a function to evaluate the total energy $E$ and Fock matrices $\{{\mathbf{F}}_p^{\sigma }\}$ for a given set of orbitals $\{{\mathbf{C}}_p^{\sigma }\}$. The only assumption behind the library is that one is able to easily store Fock and orbital matrices in memory, and to diagonalize the Fock matrices in full, which is the case in the overwhelming majority of quantum chemistry applications. We exemplify the library with nuclear-electronic orbital (NEO) calculations of protonated water clusters with Gaussian-type orbital basis sets. We find that a minimal-basis protonic guess works well, and that the stepwise SCF algorithm requires less computational time than the simultaneous SCF algorithm.

26 pages

References in corpus (27)

• Recent developments in the PySCF program package
• Development of a Practical Multicomponent Density Functional for Electron-Proton Correlation to Produce Accurate Proton Densities
• ELSI: A Unified Software Interface for Kohn-Sham Electronic Structure Solvers
• An assessment of initial guesses for self-consistent field calculations. Superposition of Atomic Potentials: simple yet efficient
• An overview of self-consistent field calculations within finite basis sets
• A review on non-relativistic fully numerical electronic structure calculations on atoms and diatomic molecules
• ELSI -- An Open Infrastructure for Electronic Structure Solvers
• Fully numerical calculations on atoms with fractional occupations. Range-separated exchange functionals
• Fully numerical Hartree-Fock and density functional calculations. I. Atoms
• Straightforward and accurate automatic auxiliary basis set generation for molecular calculations with atomic orbital basis sets
• Meta-GGA density functional calculations on atoms with spherically symmetric densities in the finite element formalism
• Fully numerical electronic structure calculations on diatomic molecules in weak to strong magnetic fields
• Communication: Curing basis set overcompleteness with pivoted Cholesky decompositions
• The CECAM Electronic Structure Library and the modular software development paradigm
• Efficient implementation of the superposition of atomic potentials initial guess for electronic structure calculations in Gaussian basis sets
• A call to arms: making the case for more reusable libraries
• Atomic electronic structure calculations with Hermite interpolating polynomials
• Fully numerical Hartree-Fock and density functional calculations. II. Diatomic molecules
• On the accurate reproduction of strongly repulsive interatomic potentials
• The orbital minimization method for electronic structure calculations with finite-range atomic basis sets
• Automatic Generation of Accurate and Cost-efficient Auxiliary Basis Sets
• Convergence analysis of adaptive DIIS algorithms with application to electronic ground state calculations
• Second-order self-consistent field algorithms: from classical to quantum nuclei
• Economical Quasi-Newton Self Consistent Field Solver
• Insight on Gaussian basis set truncation errors in weak to intermediate magnetic fields with an approximate Hamiltonian
• OpenOrbitalOptimizer -- a reusable open source library for self-consistent field calculations
• Systematic study of confinement induced effects on atomic electronic structure

Cited by in corpus (6)

• OpenOrbitalOptimizer -- a reusable open source library for self-consistent field calculations
• The Enduring Relevance of Semiempirical Quantum Mechanics
• Reaching precise proton affinities in non-Born-Oppenheimer calculations
• A Reusable Library for Second-Order Orbital Optimization Using the Trust Region Method
• Atomic Confinement Potentials and the Generation of Numerical Atomic Orbitals
• libwignernj: a reusable C/C++/Fortran/Python library for exact Wigner symbols and related coefficients