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Updated: Apr 26, 2026

Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry
Published on: April 8, 2020
Communication: Relativistic Fock-space coupled cluster study of small building blocks of larger uranium complexes
Paweł Tecmer1, André Severo Pereira Gomes2, Stefan Knecht3
1Amsterdam Center for Multiscale Modeling (ACMM), VU University Amsterdam, De Boelelaan 1083, 1081 HV Amsterdam, The Netherlands.
Abstract:
We present a study of the electronic structure of the [UO2](+), [UO2](2 +), [UO2](3 +), NUO, [NUO](+), [NUO](2 +), [NUN](-), NUN, and [NUN](+) molecules with the intermediate Hamiltonian Fock-space coupled cluster method. The accuracy of mean-field approaches based on the eXact-2-Component Hamiltonian to incorporate spin-orbit coupling and Gaunt interactions are compared to results obtained with the Dirac-Coulomb Hamiltonian. Furthermore, we assess the reliability of calculations employing approximate density functionals in describing electronic spectra and quantities useful in rationalizing Uranium (VI) species reactivity (hardness, electronegativity, and electrophilicity).
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