Full metadata record
DC FieldValueLanguage
dc.contributor.authorKOVACS ATTILAen_GB
dc.contributor.authorKONINGS Rudyen_GB
dc.date.accessioned2012-01-13T01:01:44Z-
dc.date.available2012-01-11en_GB
dc.date.available2012-01-13T01:01:44Z-
dc.date.created2012-01-11en_GB
dc.date.issued2011en_GB
dc.date.submitted2011-03-29en_GB
dc.identifier.citationJOURNAL OF PHYSICAL CHEMISTRY A vol. 115 no. 24 p. 6646 – 6656en_GB
dc.identifier.issn1089-5639en_GB
dc.identifier.urihttp://pubs.acs.org/doi/abs/10.1021/jp202538ken_GB
dc.identifier.urihttp://publications.jrc.ec.europa.eu/repository/handle/JRC64469-
dc.description.abstractThe vibrational frequencies of the actinide oxides AnO and AnO2 (An = Th, Pa, U, Np, Pu, Am, Cm) and of their mono- and dications have been calculated using advanced quantum chemical techniques. The stretching fundamental frequencies of the monoxides have been determined by fitting the potential function to single-point energies obtained by relativstic CASPT2 calculations along the stretching coordinate and on this basis solving numerically the ro-vibrational Schrödinger equitation. To obtain reliable fundamental frequencies of the dioxides, we developed an empirical approach. In this approach the harmonic vibrational frequencies of the AnO20/+/2+ species were calculated using eight different exchange-correlations DFT functional. On the basis of the good correlation found between the vibrational frequencies and computed bond distances, the final frequency values were derived for the CASPT2 reference bond distances from linear regression equitations fitted to the DFT data of each species, As test, the approach provided excellent agreement with accurate experimental data of ThO, ThO+, UO and UO+. The joint analysis of literature experimental and our computed data facilitated the prediction of reliable gas-phase molecular properties for some oxides. They include the stretching frequencies of PuO, ThO2, Uo2 and Uo2+ and the bond distance of PuO (1.818 Å. being likely within 0.002 Å of the real value). Also the derived equilibrium bond distances of ThO2, UO2 and UO2+ (1.896, 1.790 and 1.758 Å, respectively) should approximate closely the (yet unknown) experimental values. On the basis of the present results we suggest that the ground electronic state of PuO2 in Ar and Kr matrices is probably different from that in the gaseous phase, similarly to UO2 observed previously.en_GB
dc.description.sponsorshipJRC.E.3-Materials researchen_GB
dc.format.mediumPrinteden_GB
dc.languageENGen_GB
dc.publisherAMER CHEMICAL SOCen_GB
dc.relation.ispartofseriesJRC64469en_GB
dc.titleComputed vibrational frequencies of actinide oxides AnO0/+/2+ and AnO20/+/2+ (An = Th, Pa, U, Np, Pu, Am, Cm)en_GB
dc.typeArticles in periodicals and booksen_GB
dc.identifier.doi10.1021/jp202538ken_GB
JRC Directorate:Nuclear Safety and Security

Files in This Item:
There are no files associated with this item.


Items in repository are protected by copyright, with all rights reserved, unless otherwise indicated.