Structure of Stoichiometric and Oxygen-Rich Ultrathin FeO(111) Films Grown on Pd(111)

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Abstract

Monolayer thin FeO(111) films were grown on Pd(111) and oxidized by atomic oxygen (O). The stoichiometric and oxidized films were studied in detail by scanning tunneling microscopy (STM) and density functional theory (DFT) calculations. Compared to the previously studied FeO(111)/Pt(111) system, small structural differences were observed for stoichiometric FeO monolayer films. Upon O exposure, the stoichiometric FeO film reconstructs, leading to the formation of new O-rich structures incorporating increasing amounts of additional O atoms. At low O exposures, the STM images exhibit bright features of regularly sized triangular structures assigned to O-adatom dislocation loops. A model of this O-rich structure composed of four-fold O-coordinated Fe atoms is proposed and confirmed by DFT calculations. Furthermore, these O dislocation loops induce the inversion of the FeO film and enclose portions of the film in which the order of the high-symmetry domains is inverted. For higher O exposures, the formation of FeO2–x islands coexisting with O-adatom dislocations and stoichiometric FeO patches was observed. These FeO2–x islands are reminiscent of the O-rich structures previously reported for FeO supported on Pt(111) and are catalytically active toward CO oxidation.

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