1. Plasmonic Hot Electron Transport Driven Site-Specific Surface-Chemistry with Nanoscale Spatial Resolution
- Author
-
Cort��s, Emiliano, Xie, Wei, Cambiasso, Javier, Jermyn, Adam S., Sundararaman, Ravishankar, Narang, Prineha, Schl��cker, Sebastian, and Maier, Stefan A.
- Subjects
Chemical Physics (physics.chem-ph) ,Condensed Matter::Materials Science ,Condensed Matter - Mesoscale and Nanoscale Physics ,Physics - Chemical Physics ,Mesoscale and Nanoscale Physics (cond-mat.mes-hall) ,FOS: Physical sciences ,Physics::Optics ,Optics (physics.optics) ,Physics - Optics - 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 nanometre 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 hot-carrier extraction science and nanoscale regio-selective surface chemistry., 18 pages, 5 figures
- Published
- 2016