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Abstract

We studied the preparation of thin silica films on Pd(111) using low energy electron diffraction (LEED), infrared reflection-absorption spectroscopy (IRAS), and scanning tunneling microscopy (STM). The films grow from the onset as a double-layer (bilayer) silicate and show no long-range ordering as judged by LEED, thus bearing close similarities to the silicate films grown on a Pt(111) support. The results provide further evidence that the principal structure (monolayer vs bilayer) of ultrathin silica films on metal substrates is primarily governed by the affinity of a metal substrate to oxygen. Individual adsorption of CO and D₂ on the prepared films showed that both molecules penetrate through the film and chemisorb on the Pd(111) surface. Density functional theory (DFT) calculations showed that CO bonding on Pd(111) underneath the silica film becomes weaker as compared to the bare Pd(111) surface, but the vibrational frequencies remain unaffected, that is in nice agreement with the experimental results.