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

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

doi:10.1063/5.0135089

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

Journal Article · Wed Feb 22 00:00:00 EST 2023 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0135089· OSTI ID:1958268

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^[1]; Withanage, Kushantha K. ^[1];

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^[1]; Khandal, Kusal ^[1]; Lasode, Peter O. ^[1];

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^[2]

Univ. of Texas at El Paso, TX (United States)
Central Michigan Univ., Mount Pleasant, MI (United States)

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 2^N – 2 initial starting points for systems composed of a smaller number of electrons. As a result, applications to heavy and super-heavy atoms are presented. All starting solutions reported here were obtained from a solution for element 118, Oganesson.

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Research Organization:: Central Michigan Univ., Mount Pleasant, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE

Grant/Contract Number:: SC0018331; SC0019330; 209668; NM1103

OSTI ID:: 1958268

Alternate ID(s):: OSTI ID: 1958237

Journal Information:: Journal of Chemical Physics, Vol. 158, Issue 8; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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

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