A Theoretical Characterization of Covalency in Rare Earth Complexes through Their Absorption Electronic Properties: f-f Transitions
Experimental uncertainties concerning the coordination mode of trivalent plutonium in concentrated LiCl have led us to theoretically evaluate the f-f transitions of a series of rare earth aquo and chloro complexes. The calculation of Pr(III), U(III), Np(III), and Pu(III) systems' spectra was undertaken using the LFDFT (ligand field density functional theory) route that combines the backgrounds of ligand field (LF) theory with Kohn-Sham orbitals. LF parameters are fitted to previous DFT calculations, thus preventing the use of empirical data. The f-f transitions values are globally well predicted, but the lack of accurate experimental references can sometimes hinder reliable comparisons. Despite this, the nephelauxetic effect from aquo to chloro complexes is clearly observed through both spectral red shifts and the decrease in F2, the Slater-Condon parameter. Accordingly, this work provides the first theoretical characterization of covalency in trivalent f elements through their electronic spectra.
WOS:000240033700048
2006
45
18
7382
7388
REVIEWED