Reaction of Laser-Ablated Uranium and Thorium Atoms with H2Se: A Rare Example of Selenium Multiple Bonding.

Abstract

The compounds H2ThSe and H2USe were synthesized by the reaction of laser-ablated actinide metal atoms with H2Se under cryogenic conditions following the procedures used to synthesize H2AnX (An = Th, U; X = O, S). The molecules were characterized by infrared spectra in an argon matrix with the aid of deuterium substitution and electronic structure calculations at the density functional theory level. The main products, H2ThSe and H2USe, are shown to have a highly polarized actinide-selenium triple bond, as found for H2AnS on the basis of electronic structure calculations. There is an even larger back-bonding of the Se with the An than found for the corresponding sulfur compounds. These molecules are of special interest as rare examples of multiple bonding of selenium to a metal, particularly an actinide metal.