A new generation of effective core potentials: Selected lanthanides and heavy elements

Zhou, Haihan; Kincaid, Benjamin; Wang, Guangming; Annaberdiyev, Abdulgani; Ganesh, Panchapakesan; Mitas, Lubos

doi:10.1063/5.0180057

Title: A new generation of effective core potentials: Selected lanthanides and heavy elements

Journal Article · 22 February 2024 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0180057 · OSTI ID:2317750

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North Carolina State University, Raleigh, NC (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Here, we construct correlation-consistent effective core potentials (ccECPs) for a selected set of heavy atoms and ƒ-elements that are of significant current interest in materials and chemical applications, including Y, Zr, Nb, Rh, Ta, Re, Pt, Gd, and Tb. As is customary, ccECPs consist of spin orbit averaged relativistic effective potential (AREP) and effective spin-orbit (SO) terms. For the AREP part, our constructions are carried out within a relativistic coupled-cluster framework while also taking into account objective function one-particle characteristics for improved convergence in optimizations. The transferability is adjusted using binding curves of hydride and oxide molecules. We address the difficulties encountered with ƒ-elements, such as the presence of large cores and multiple near-degeneracies of excited levels. For these elements, we construct ccECPs with core valence partitioning that includes 4ƒ-subshell in the valence space. The developed ccECPs achieve an excellent balance between accuracy, size of the valence space, and transferability and are also suitable to be used in plane wave codes with reasonable energy cutoffs.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 2317750

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 8 Vol. 160; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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