“…[1] Defect formation and void swelling in UO 2 fuel pellets dramatically reduce the lifetime and energy output of these materials,b ut the direct study of the surface oxidation processes that cause these defects can be challenging due to the chemical complexity and extreme radioactivity of spent fuels. [1][2][3] Due to their large active surface areas,phase-pure UO 2 thin films can serve as an excellent model systems for the chemical and physical changes that occur at the grain boundaries of bulk UO 2 fuel pellets.U ranium oxide thin films have been fabricated using both solution [4][5][6] and sputtering [7][8][9][10] methods;h owever,a chieving stoichiometric control in the resulting films has been challenging due to the wide array of accessible uranium oxide phases and the facile interconversion of these phases at grain boundaries. [5,11] Consequently,m any published studies on uranium oxide have been performed using materials with avarying degree of amorphous or polycrystalline character.…”