Downward quantum learning from element 118: Automated generation of Fermi-Löwdin orbitals for all atoms

Mark R. Pederson, Alexander I. Johnson, Kushantha P.K. Withanage, Sherab Dolma, Gustavo Bravo Flores, Zahra Hooshmand, Kusal Khandal, Peter O. Lasode, Tunna Baruah, Koblar A. Jackson

Research output: Contribution to journalArticlepeer-review


A new algorithm based on a rigorous theorem and quantum data computationally mined from element 118 guarantees automated construction of initial Fermi-Löwdin-Orbital (FLO) starting points for all elements in the Periodic Table. It defines a means for constructing a small library of scalable FLOs for universal use in molecular and solid-state calculations. The method can be systematically improved for greater efficiency and for applications to excited states such as x-ray excitations and optically silent excitations. FLOs were introduced to recast the Perdew-Zunger self-interaction correction (PZSIC) into an explicit unitarily invariant form. The FLOs are generated from a set of N quasi-classical electron positions, referred to as Fermi-Orbital descriptors (FODs), and a set of N-orthonormal single-electron orbitals. FOD positions, when optimized, minimize the PZSIC total energy. However, creating sets of starting FODs that lead to a positive definite Fermi orbital overlap matrix has proven to be challenging for systems composed of open-shell atoms and ions. The proof herein guarantees the existence of a FLOSIC solution and further guarantees that if a solution for N electrons is found, it can be used to generate a minimum of N - 1 and a maximum of 2N - 2 initial starting points for systems composed of a smaller number of electrons. Applications to heavy and super-heavy atoms are presented. All starting solutions reported here were obtained from a solution for element 118, Oganesson.

Original languageEnglish
Article number084101
JournalJournal of Chemical Physics
Issue number8
StatePublished - Feb 28 2023


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