Abstract
We use surface second harmonic generation spectroscopy (s-SHG) to study the oxidation of supported, size-selected silver clusters under ultra-high vacuum conditions. The oxidation reaction of small silver clusters between \(\hbox {Ag}_{9}\) and \(\hbox {Ag}_{55}\) is monitored by means of their localized surface plasmon resonance. We observe a rapid decline of the SH-intensity, as soon as cluster samples are exposed to an oxygen partial pressure of \(5 \times 10^{-6}\) mbar, which is attributed to the formation of silver–oxygen-bonds. The evolution of the SH-intensity under exposure to oxygen shows a double-exponential character for all investigated cluster sizes. Since the oxidation of single crystalline silver surfaces follow single-exponential Langmuir-kinetics, the two independent pathways of SH-intensity loss are attributed to a surface- and an interface-oxidation of supported clusters, respectiveley. For small cluster sizes, a complete loss of the SH intensity is obtained, which suggests the complete oxidation of the clusters. For larger clusters a plasmonic resonance is still observed after oxidation, indicating a residual free-electron density.
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This work has been supported by the BMBF through the project IC4, the European Research Council through an Advanced Research Grant (246645-ASC3), and the DFG through the Project (HE 3454/21-1).
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Lünskens, T., Walenta, C.A., Heister, P. et al. Surface Oxidation of Supported, Size-Selected Silver Clusters. J Clust Sci 28, 3185–3192 (2017). https://doi.org/10.1007/s10876-017-1285-y
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DOI: https://doi.org/10.1007/s10876-017-1285-y