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Nano Lett. 2012 Mar 14;12(3):1333-9. doi: 10.1021/nl300269c. Epub 2012 Feb 14.

Quantum plasmonics: nonlinear effects in the field enhancement of a plasmonic nanoparticle dimer.

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Institut des Sciences Moléculaires d'Orsay, UMR 8214 CNRS-Université Paris-Sud, Bâtiment 351, 91405 Orsay Cedex, France.


A fully quantum mechanical investigation using time-dependent density functional theory reveals that the field enhancement in a coupled nanoparticle dimer can be strongly affected by nonlinear effects. We show that both classical as well as linear quantum mechanical descriptions of the system fail even for moderate incident light intensities. An interparticle current resulting from the strong field photoemission tends to neutralize the plasmon-induced surface charge densities on the opposite sides of the nanoparticle junction. Thus, the coupling between the two nanoparticles and the field enhancement is reduced as compared to linear theory. A substantial nonlinear effect is revealed already at incident powers of 10(9) W/cm(2) for interparticle separation distances as large as 1 nm and down to the touching limit.

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