4.7 Article

A new generation of effective core potentials from correlated and spin-orbit calculations: Selected heavy elements

期刊

JOURNAL OF CHEMICAL PHYSICS
卷 157, 期 5, 页码 -

出版社

AIP Publishing
DOI: 10.1063/5.0087300

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资金

  1. U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
  2. National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility [DE-AC02-05CH11231]
  3. DOE Office of Science User Facility [DE-AC02-06CH11357, DE-AC05-00OR22725]
  4. Center for Predictive Simulation of Functional Materials
  5. US Department of Energy (DOE) [DE-AC05-00OR22725]

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This study introduces new correlation consistent effective core potentials (ccECPs) for several elements, which provide a significant increase in accuracy for valence-only calculations. The importance of the AREP part in determining the overall quality of the ECP is confirmed.
We introduce new correlation consistent effective core potentials (ccECPs) for the elements I, Te, Bi, Ag, Au, Pd, Ir, Mo, and W with 4d, 5d, 6s, and 6p valence spaces. 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, norm-conservation criteria, and SO 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. The subsequent quantum Monte Carlo calculations point out the importance of accurate trial wave functions that, in some cases (mid-series transition elements), require treatment well beyond a single-reference. Published under an exclusive license by AIP Publishing.

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