A MATRIX-ISOLATION FT-IR AND QUASI-RELATIVISTIC DENSITY-FUNCTIONAL THEORY INVESTIGATION OF THE REACTION-PRODUCTS OF LASER-ABLATED URANIUM ATOMS WITH NO, NO2 AND N2O

The reaction products of laser-ablated uranium atoms with nitrogen oxi de reagent gases were trapped in excess argon at 6-7 K. Infrared spect ra of the resulting matrices revealed the presence of several new prod uct species. Major bands at 983.6 and 818.9 cm(-1) in the infrared spe ctra of the reaction products of U atoms with (NO)-N-14-O-16 are due t o the U-N and U-O stretching vibrations, respectively, of the linear N UO molecule. Weaker absorptions at 845.9 cm(-1) and 718.3 cm(-1) in si milar experiments are indicative of a ''T'' shaped NUO2 species. A wea ker 1017.0 cm(-1) band provides evidence for the cation/anion pair [NU O](+)[NO](-). Several possible products of the reaction of uranium ato ms with nitrogen oxides have been further characterized by quasirelati vistic density functional calculations. (C) 1997 American Institute of Physics.