A Reusable Library for Second-Order Orbital Optimization Using the Trust Region Method
arXiv:2509.13931 · doi:10.1021/acs.jctc.5c01576
Abstract
We present a reusable, open-source software implementation of the second-order trust region algorithm in the new OpenTrustRegion library. We apply the implementation to the general-purpose optimization of molecular orbitals in various contexts within electronic-structure theory. Our permissibly licensed implementation can be included in any software package, be it free and open-source, academically licensed closed-source, or commercial. Detailing the implementation in OpenTrustRegion, we present a review of the theory behind trust region-based methods alongside various extensions. We demonstrate the robustness and efficiency of our optimization library with extensive benchmarks for self-consistent field calculations, orbital localization, as well as orbital symmetrization tasks, featuring challenging and pathological systems.
31+20 pages, 5 figures. SI and selected geometries as ancillary files
References in corpus (24)
- Recent developments in the PySCF program package
- NWChem: Past, Present, and Future
- Real-Space Mesh Techniques in Density Functional Theory
- Daubechies wavelets as a basis set for density functional pseudopotential calculations
- Excited state orbital optimization via minimizing the square of the gradient: General approach and application to singly and doubly excited states via density functional theory
- eT 1.0: an open source electronic structure program with emphasis on coupled cluster and multilevel methods
- A general second order complete active space self-consistent-field solver for large-scale systems
- An assessment of initial guesses for self-consistent field calculations. Superposition of Atomic Potentials: simple yet efficient
- A review on non-relativistic fully numerical electronic structure calculations on atoms and diatomic molecules
- A trust-region augmented Hessian implementation for restricted and unrestricted Hartree-Fock and Kohn-Sham methods
- Fully numerical calculations on atoms with fractional occupations. Range-separated exchange functionals
- Theory and applications of generalized Pipek--Mezey Wannier functions
- Large-scale relativistic complete active space self-consistent field with robust convergence
- 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
- Hybrid grid/basis set discretizations of the Schrödinger equation
- Orbital optimization in the perfect pairing hierarchy. Applications to full-valence calculations on linear polyacenes
- Second-order self-consistent field algorithms: from classical to quantum nuclei
- A black-box, general purpose quadratic self-consistent field code with and without Cholesky Decomposition of the two-electron integrals
- Economical Quasi-Newton Self Consistent Field Solver
- OpenOrbitalOptimizer -- a reusable open source library for self-consistent field calculations
- Riemannian Trust Region Method for Minimization of Fourth Central Moment for Localized Molecular Orbitals
- Symmetrization of Localized Molecular Orbitals
- Coupled-cluster pairing models for radicals with strong correlations