This website uses cookies to give you the best user experience. If you continue
without changing your settings we'll assume you are happy to receive all RSC cookies.
You can change your cookie settings by navigating to our Privacy and Cookies page and following the instructions. These instructions
are also obtainable from the privacy link at the bottom of any RSC page.
We report density functional calculations of the surface properties and chemistry of UO2(111) performed within the generalized gradient approximation corrected with an effective Hubbard parameter (GGA + U within Dudarev's formalism) to account for the strong on-site Coulomb repulsion between U 5f electrons. The variation of the properties of periodic slab models, with collinear ferromagnetic and antiferromagnetic arrangements of the uranium magnetic moments, was investigated while ramping up the effective Hubbard parameter from Ueff = 0 eV, corresponding to standard density functional theory, up to Ueff = 4 eV, the value that correctly reproduces the antiferromagnetic ground state of bulk UO2. The chemical interactions of molecular water, dissociated water, dissociated oxygen and co-adsorbed molecular water and monatomic oxygen with the UO2(111) surface were also studied as functions of the Ueff parameter. Calculations reveal that some of the key electronic and chemical properties controlling the surface reactivity are very sensitive to the value of this strong electron correlation parameter.
Fetching data from CrossRef. This may take some time to load.