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Subnanometric plasmonics: confining light to atomic-scale dimensions

AutorAizpurua, Javier ; Barbry, Marc; Koval, P. ; Marchesin, Federico ; Esteban, Ruben; Borisov, Andrei G.; Sánchez-Portal, Daniel
Fecha de publicación2015
CitaciónPACIFICHEM 2015
ResumenPlasmonic fields have boosted field-enhanced spectroscopy and microscopy due to their effective antenna action improving both the field enhancement, as well as producing useful nanometric localization. As novel geometrical architectures are being developed in plasmonic gap configurations, subnanometric separation distances and features become a common situation that needs to be addressed to understand the performance of extreme field-enhanced spectroscopy. We theoretically analyze the optical response of ultranarrow plasmonic gaps, such as those in nanoparticle on mirror (NPoM) configurations, or in cavities of tip-enhanced Raman scattering (TERS), where a rich variety of complex optoelectronic processes emerge due to the subnanometric nature of the architectures involved. By a combination of classical electrodynamical and quantum mechanical calculations, we are able to reveal a complex distribution of modes in the optical response of the cavities with hybridizations and strong nonlinear effects affecting the ultimate limits of light confinement. We present state-of-the-art quantum mechanical calculations that reveal atomic-scale localization in plasmonic structures, given by the presence of crystallographic facets, vertices, and edges. These features produce an analogue to an atomistic lightning rod effect that further enhances the underlying nanometric plasmon near-field in a cascade effect, scaled down to atomic dimensions. The implications of atomic-scale localization of light in the optical resolution of field-enhanced spectroscopies, photochemistry and photoemission can be dramatic and might explain the tremendous variability of experimental findings.
DescripciónResumen del trabajo presentado al International Chemical Congress of Pacific Basin Societies, celebrado en Honolulu, Hawai (USA) del 15 al 20 de diciembre de 2015.
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