Accuracy of relativistic energy-consistent pseudopotentials for superheavy elements 111-118: Molecular calibration calculations

Journal Article · Mon Jan 28 00:00:00 EST 2013 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4776757· OSTI ID:22105341

Hangele, Tim; Dolg, Michael ^[1]

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1. Institute for Theoretical Chemistry, University of Cologne, Greinstr. 4, 50939 Cologne (Germany)

Relativistic energy-consistent pseudopotentials modelling the Dirac-Coulomb-Breit Hamiltonian with a finite nucleus model for the superheavy elements with nuclear charges 111-118 were calibrated in atomic and molecular calculations against fully relativistic all-electron reference data. Various choices for the adjustment of the f-potentials were investigated and an improved parametrization is recommended. Using the resulting pseudopotentials relativistic all-electron reference data can be reproduced at the self-consistent field level with average absolute (relative) errors of 0.0030 A (0.15%) for bond lengths and 2.79 N m{sup -1} (1.26%) for force constants for 24 diatomic test molecules, i.e., neutral or singly charged monohydrides, monofluorides, and monochlorides with closed-shell electronic structure. At the second-order Moller-Plesset perturbation theory level the corresponding average deviations are 0.0033 A (0.15%) for bond lengths and 2.86 N m{sup -1} (1.40%) for force constants. Corresponding improved f-potentials were also derived for the pseudopotentials modelling in addition the leading contributions from quantum electrodynamics.

• OSTI ID: 22105341
• Journal Information: Journal of Chemical Physics, Vol. 138, Issue 4; Other Information: (c) 2013 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
73 NUCLEAR PHYSICS AND RADIATION PHYSICS
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ACCURACY
BOND LENGTHS
CALIBRATION
ELECTRONIC STRUCTURE
HAMILTONIANS
HEAVY NUCLEI
PERTURBATION THEORY
POTENTIALS
QUANTUM ELECTRODYNAMICS
RELATIVISTIC RANGE
SELF-CONSISTENT FIELD
SIMULATION
TRANSACTINIDE ELEMENTS