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Study of Heavy Elements by Relativistic Fock Space and Intermediate Hamiltonian Coupled Cluster Methods

  • Chapter
Fundamental World of Quantum Chemistry

Abstract

High-accuracy ground- and excited-state energies of heavy and superheavy atoms are calculated in the framework of the Dirac-CoulombBreit Hamiltonian. Electron correlation is treated by the Fock-space coupled cluster method. Several variants of the recently developed intermediate Hamiltonian approach are also described. These schemes make possible much larger P (model) spaces, which may be varied to convergence without encountering intruder state problems, thus enhancing accuracy and allowing application to states not accessible before. In particular, the mixed-sector IH scheme suppresses intruder states coming from higher Fock space sectors, making it possible to use quasi-closed shells (p2, d4 etc.) as reference. Very large basis sets, going up to l= 8, are used. The outer 20–40 electrons are correlated. Representative applications are described, showing excellent agreement with experimentally known transition energies of heavy atoms, usually within a few hundredths of an eV. This makes possible reliable predictions for superheavy elements, found to possess chemical and spectroscopic properties significantly different from their lighter homologues.

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Authors and Affiliations

  1. School of Chemistry, Tel Aviv University, 69551, Tel Aviv, Israel

    Uzi Kaldor, Ephraim Eliav & Arie Landau

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  1. Uzi Kaldor
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Editors and Affiliations

  1. Uppsala University, Uppsala, Sweden

    Erkki J. Brändas

  2. Bogoliubov Institute for Theoretical Physics, Kiev, Ukraine

    Eugene S. Kryachko

  3. University of Leuven, Leuven, Belgium

    Eugene S. Kryachko

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Kaldor, U., Eliav, E., Landau, A. (2004). Study of Heavy Elements by Relativistic Fock Space and Intermediate Hamiltonian Coupled Cluster Methods. In: Brändas, E.J., Kryachko, E.S. (eds) Fundamental World of Quantum Chemistry. Springer, Dordrecht. https://doi.org/10.1007/978-94-017-0448-9_17

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  • DOI: https://doi.org/10.1007/978-94-017-0448-9_17

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