Plasmonic hot electron transport drives nano-localized chemistry

Emiliano Cortés (), Wei Xie, Javier Cambiasso, Adam S. Jermyn, Ravishankar Sundararaman, Prineha Narang (), Sebastian Schlücker () and Stefan A. Maier
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Emiliano Cortés: The Blackett Laboratory, Imperial College London
Wei Xie: Physical Chemistry I, University of Duisburg-Essen
Javier Cambiasso: The Blackett Laboratory, Imperial College London
Adam S. Jermyn: Institute of Astronomy, Cambridge University
Ravishankar Sundararaman: Rensselaer Polytechnic Institute
Prineha Narang: Faculty of Arts and Sciences, Harvard University
Sebastian Schlücker: Physical Chemistry I, University of Duisburg-Essen
Stefan A. Maier: The Blackett Laboratory, Imperial College London

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications of plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded the scope of plasmonic applications to exploit the generated hot carriers. However, quantitative understanding of the spatial localization of these hot carriers, akin to electromagnetic near-field maps, has been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution as a function of time and electromagnetic field polarization for different plasmonic nanostructures. We combine experiments employing a six-electron photo-recycling process that modify the terminal group of a self-assembled monolayer on plasmonic silver nanoantennas, with theoretical predictions from first-principles calculations of non-equilibrium hot-carrier transport in these systems. The resulting localization of reactive regions, determined by hot-carrier transport from high-field regions, paves the way for improving efficiency in hot-carrier extraction science and nanoscale regio-selective surface chemistry.

Date: 2017
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DOI: 10.1038/ncomms14880

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