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Augmented Roothaan-Hall Hessian Applied to Spin-Restricted Open-Shell Density-Functional Theory

arXiv:2606.03709v1 Announce Type: new Abstract: We generalize the augmented Roothaan-Hall (ARH) Hessian formalism to the self-consistent field (SCF) optimization of spin-restricted open-shell (RO) wavefunctions, encompassing high-spin, low-spin, and two-determinant electronic states. A detailed ARH formulation is presented. We demonstrate that ARH is a highly efficient optimization algorithm for rapidly identifying accurate SCF minima, primarily owing to its systematic construction of an...

arXiv Physics 7d ago