NANOSYSTEMS: PHYSICS, CHEMISTRY, MATHEMATICS, 2014, 5 (4), P. 494-508
ELECTRONIC STRUCTURE AND STABILIZATION OF C60 FULLERENES ENCAPSULATING ACTINIDE ATOM
M. V. Ryzhkov – Institute of Solid State Chemistry, Ural Branch of the Russian Academy of Sciences, 620990, Ekaterinburg, Russia; ryz@ihim.uran.ru
A. L. Ivanovskii – Institute of Solid State Chemistry, Ural Branch of the Russian Academy of Sciences, 620990, Ekaterinburg, Russia
B. Delley – Paul Scherrer Institut WHGA 123, CH-5232, Villigen PSI, Switzerland
The geometry optimization of the neutral molecules An@C60 (An = Th – Md) was carried out using the DFT based Dmol3 method. In order to perform calculations for these complexes’ electronic structures, the fully relativistic discrete variational method (RDV) was used. Two types of stable position of metal atom inside
the C60 cage were obtained. The most stable non-central positions are favored over the position of actinide in the fullerene center for all An@C60 complexes. Systems containing light actinides have considerable energetic stability, which is noticeably greater than that of corresponding exohedral and “networked” complexes. The 5f-orbitals’ contribution to chemical bonding was found to be noticeably less than that of the 6d-states, even for the complexes at the beginning of An@C60 row. The e ective charges on the actinide atoms were calculated using integral scheme incorporated in RDV and Hirshfeld procedure of DMol3 code.
Keywords: fullerenes, actinides, ab initio methods, relativistic calculations, molecular structure, stability.
PACS 31.15A, 31.15ae, 31.15aj, 31.15E
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