Mass Spectrum and Theoretical Calculation for Azide Radical Complexes With Uranyl(Ⅴ) Cation ［UO2(N3)n］+(n=1-4)

Coordination of uranium chemistry by multiligands has attracted attention as a way to obtain unique molecular structures and their possible use in environmental and nuclear waste disposal. In this work, mass spectrum with positive ions ［UO2(N3)n］+(n=0-4) as the dominant peaks generated by laser evaporation of uranium target with N2O as the carrier gas is reported. The associated quantitative calculations are carried out to explore structures and bonding interactions. The calculations show that N3 is bound to UO+2 as a radical and reveal that the bonding interaction in the whole system is found only between the first N3 ligand and uranium atom. Further localized molecular orbital analyses indicate the presence of multi-centered orbital delocalization in the system.