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Relativistic coupled cluster study of diatomic compounds of Hg, Cn, and Fl

Borschevsky, A., Pershina, V., Eliav, E. & Kaldor, U., 28-Aug-2014, In : Journal of Chemical Physics. 141, 8, 7 p., 084301.

Research output: Contribution to journalArticleAcademicpeer-review

The structure and energetics of eight diatomic heavy-atom molecules are presented. These include the species MAu, M-2, and MHg, with M standing for the Hg, Cn (element 112), and Fl (element 114) atoms. The infinite-order relativistic 2-component Hamiltonian, known to closely reproduce 4-component results at lower computational cost, is used as framework. High-accuracy treatment of correlation is achieved by using the coupled cluster scheme with single, double, and perturbative triple excitations in large converged basis sets. The calculated interatomic separation and bond energy of Hg-2, the only compound with known experimental data, are in good agreement with measurements. The binding of Fl to Au is stronger than that of Cn, predicting stronger adsorption on gold surfaces. The bond in the M-2 species is strongest for Fl(2), being of chemical nature; weaker bonds appear in Cn(2) and Hg-2, which are bound by van der Waals interactions, with the former bound more strongly due to the smaller van der Waals radius. The same set of calculations was also performed using the relativistic density functional theory approach, in order to test the performance of the latter for these weakly bound systems with respect to the more accurate coupled cluster calculations. It was found that for the MAu species the B3LYP functional provides better agreement with the coupled cluster results than the B88/P86 functional. However, for the M2 and the MHg molecules, B3LYP tends to underestimate the binding energies. (C) 2014 AIP Publishing LLC.

Original languageEnglish
Article number084301
Number of pages7
JournalJournal of Chemical Physics
Volume141
Issue number8
Publication statusPublished - 28-Aug-2014
Externally publishedYes

    Keywords

  • ELECTRONIC-STRUCTURE, HEAVIEST ELEMENTS, HEAVY-ELEMENTS, METAL-SURFACES, SPIN-ORBIT, DENSITY, TRANSITION, MERCURY, EXCHANGE, APPROXIMATION

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