Photoexcitation of the surface plasmon resonance (SPR) in noble metal nanoparticles results in the production of a strong electric field, high-energy electrons, and high temperatures at the nanoparticle surface.  There have been demonstrations utilizing each of these effects to perform chemical reactions; however, there is currently no detailed understanding of the relative spatial-temporal relevance of these effects for chemical reactivity. To elucidate the time and space dependence of the above effects, we use the Woodward-Hoffman rules to design chemical probes that proceed by only one of the three mechanisms.  These probes are anchored to the nanoparticle surface at varying distances from the surface.  By monitoring the reaction process with ultrafast infrared spectroscopy, we develop a spatial and temporal map of the effects of surface plasmon excitation, in terms of chemical reactivity. This map will provide a means to efficiently and selectively control plasmonic reactions.

Mapping the chemical relevance of the surface plasmon in time and space

248th National Meeting (2014)

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