Abstract
The UO4+ and UO6+ cations are produced in a supersonic molecular beam by laser vaporization and studied with infrared laser photodissociation spectroscopy using rare gas atom predissociation. The argon complexes UO4+Ar2 and UO6+Ar2 are mass-selected in a reflectron time-of-flight spectrometer and excited with an IR-OPO laser system in the range of the O-U-O and O-O stretching vibrations. These same systems are studied with computational quantum chemistry. UO4+ is found to have a central UO2 core, with an additional ?2 coordinated oxygen molecule. Charge transfer/oxidation gives the system the character of a UO 22+, O2- ion pair. UO 6+ has this same core structure, with an additional weakly bound oxygen molecule in an η1 coordination configuration. The O-U-O stretch is sensitive to the local environment and approximates the vibration of the isolated uranyl cation in these systems.
Original language | English (US) |
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Pages (from-to) | 1662-1666 |
Number of pages | 5 |
Journal | Journal of Physical Chemistry Letters |
Volume | 2 |
Issue number | 14 |
DOIs | |
State | Published - Jul 21 2011 |