A new generation of effective core potentials from correlated and spin-orbit calculations: selected transition metals and Lanthanides

ORAL

Abstract

We introduce new correlation consistent effective core potentials (ccECPs) for transition metals: Y, Zr, Nb, Rh, Ta, Re, Pt; Alkali metal: Cs; Lanthanides: Sm, Gd and Lu. For selected transition metals and Alkali metal, the s, p, and d orbital electrons with the highest and second highest principal quantum number are included in the valence space, while the valence space of Lanthanides additionally includes open-shell f-electrons. These ccECPs are given as a sum of spin-orbit averaged relativistic effective potential (AREP) and effective spin-orbit (SO) terms. The construction involves several steps with increasing refinements from more simple to fully correlated methods. The optimizations are carried out with objective functions that include weighted many-body atomic spectra and spin-orbit splittings. Transferability tests involve molecular binding curves of corresponding hydride and oxide dimers. The constructed ccECPs are systematically better and in a few cases on par with previous effective core potential (ECP) tables on all tested criteria and provide a significant increase in accuracy for valence-only calculations with these elements. Our study confirms the importance of the AREP part in determining the overall quality of the ECP even in the presence of sizable spin-orbit effects.

SNL is managed and operated by NTESS under DOE NNSA contract DE-NA0003525

*This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials.This research used resources from the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231. This research used resources from the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC02-06CH11357. This research also used resources from the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC05-00OR22725. SNL is managed and operated by NTESS under DOE NNSA contract DE-NA0003525

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Publication: A new generation of effective core potentials from correlated and spin-orbit calculations: selected transition metals and Lanthanides

Presenters

  • Haihan Zhou

    • North Carolina State University

Authors

  • Haihan Zhou

    • North Carolina State University

  • Benjamin E Kincaid

    • North Carolina State University

  • Lubos Mitas

    • North Carolina State University

  • Abdulgani Annaberdiyev

    • Oak Ridge National Lab

  • Ganesh Panchapakesan

    • Oak Ridge National Lab
    • Oak Ridge National Laboratory

  • Cody A Melton

    • Sandia National Laboratories