Ultrathin praseodymia films, which have been oxidized by molecular oxygen, have been treated additionally with oxygen plasma to increase their oxidation state. The structure and morphology of the films have been investigated by x-ray diffraction and x-ray reflectometry. Thorough analysis of these measurements gives information regarding modifications of the oxide film structure (especially the vertical lattice constants) due to the oxygen content and interface silicate formation before and after oxygen plasma treatment. Large parts of the plasma-treated samples exhibit a significantly higher oxygen content compared to the untreated samples; this is attributed to the formation of stoichiometric PrO 2 . The remaining film has only a small oxygen deficiency. Thus, a more homogeneous film structure is formed by exposure to oxygen plasma. Furthermore, no additional silicate interface formation can be detected. Rare earth oxides (REOs) are of interest for many applications in the fields of heterogeneous catalysis 1 and microelectronics.2 For instance, REO films are of potential use to improve the performance and functionality of future semiconductor devices by integrating alternative semiconductor materials into the present Si technology. 3,4 In this regard, single-crystalline REO films are under discussion as highly functional insulating buffer material to form so-called engineered Si wafers. The main research fields are integrated germanium-on-insulator systems aiming to boost the sub-45-nm complementary metal-oxide-semiconductor technologies and further to achieve the cost-effective monolithic integration of III-V optoelectronic materials (GaAs) on the Si wafer platform.Praseodymia is a promising candidate for these insulating buffer materials and previous studies show that crystalline Ge films grow epitaxially on praseodymia-silicon heterostructures.4 Since as-grown praseodymia films initially have hexagonal structure (hex-Pr 2 O 3 ), it is necessary to transform the structure of these films to PrO 2 (fluorite structure) to obtain stacking-twin-free Ge films. 4,5 For this purpose hex-Pr 2 O 3 films are usually exposed to molecular oxygen at high pressure, but full transformation to PrO 2 (111) has not been achieved yet.6-8 Instead, the films decompose into two laterally coexisting oxide species with different lattice parameters and significantly different stoichiometries (PrO 1.833 , PrO 2− ) as shown by detailed analysis of the praseodymia Bragg peaks. This is disadvantageous for the quality of the subsequently grown Ge film due to the imperfect oxygen sublattice. The thickness of an interface layer consisting of both species increases with higher annealing temperatures, too. This interface exhibits negative effects on the dielectric properties of the oxide film. Schaefer et al. 8 recently established an alternative technique to oxidize praseodymia films on Si(111) by exposure to cold oxygen plasma. Here, x-ray photoelectron spectroscopy (XPS) supported by low-energy electron diffraction (LEED) and x-ray diffract...