Palladium was vapor deposited on a thin FeO(111) film grown on a Pt(111) substrate. Scanning tunneling microscopy study has revealed that Pd wets the FeO substrate and at elevated temperatures forms extended Pd(111) monolayer islands in contrast to other oxide supports previously studied. For the first time, we have imaged the metal-oxide interface structure with atomic resolution and explained the results on the basis of ab initio calculations.

We derive a variant of a density based embedded cluster approach as an improvement to a recently proposed embedding theory for metallic substrates (Govind et al 1999 J. Chem. Phys. 110 7677; Klüner et al 2001 Phys. Rev. Lett. 86 5954). In this scheme, a local region in space is represented by a small cluster which is treated by accurate quantum chemical methodology. The interaction of the cluster with the infinite solid is taken into account by an effective one-electron embedding operator representing the surrounding region. We propose a self-consistent embedding scheme which resolves intrinsic problems of the former theory, in particular a violation of strict density conservation. The proposed scheme is applied to the well-known benchmark system CO/Pd(111).

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In this work, we investigate the intramolecular vibrational energy redistribution associated with the hydrogen transfer in a derivative of tropolone, namely 3,7-dichlorotropolone. Our quantum simulation is based on the Cartesian reaction surface Hamiltonian together with the multi-configurational time-dependent Hartree approach for the wave-packet propagation. We compare results for two model systems with 6 and 14 dimensions, respectively. The 6D model accounts for the most strongly coupled modes, whereas the 14D model includes further modes with significantly weaker couplings. The linear absorption spectrum of both models shows the development of an OH-stretching band. Furthermore the results show that despite the fact, that the additional modes in the 14D system couple significantly weaker, there are qualitative differences in the decay behavior of an OH-stretching excitation. Limitations of the present reaction surface approach are also discussed.