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RESEARCH PRODUCT
Size-Dependent Structural Evolution and Chemical Reactivity of Gold Clusters
Hannu HäkkinenUzi LandmanMichael MoselerMichael MoselerBokwon YoonBernd Von IssendorffPekka KoskinenPekka KoskinenOleg KostkoBernd A. HuberBernd A. Hubersubject
Delocalized electronGold clusterX-ray photoelectron spectroscopyChemical physicsChemistryCluster (physics)Analytical chemistryIonic bondingDensity functional theoryReactivity (chemistry)Electronic structurePhysical and Theoretical ChemistryAtomic and Molecular Physics and Opticsdescription
Ground-state structures and other experimentally relevant isomers of Au(15) (-) to Au(24) (-) clusters are determined through joint first-principles density functional theory and photoelectron spectroscopy measurements. Subsequent calculations of molecular O(2) adsorption to the optimal cluster structures reveal a size-dependent reactivity pattern that agrees well with earlier experiments. A detailed analysis of the underlying electronic structure shows that the chemical reactivity of the gold cluster anions can be elucidated in terms of a partial-jellium picture, where delocalized electrons occupying electronic shells move over the ionic skeleton, whose geometric structure is strongly influenced by the directional bonding associated with the highly localized "d-band" electrons.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2006-11-30 | ChemPhysChem |