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Nonlinear quantum tunneling effects in nanoplasmonic environments: two-photon absorption and harmonic generation

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Abstract

We use a quantum mechanical approach to derive a set of linear and nonlinear quantum conductivity coefficients for metal–insulator–metal structures with nanometer sized gaps. The immediate proximity of metallic objects generates a tunneling AC current density that endows the gap region with additional linear and nonlinear coefficients that in turn trigger linear and nonlinear absorption, and second- and third-harmonic generation. For example, a vacuum gap approximately 0.8 nm thick displays an effective |χ(2)|0.1pm/V for adjacent objects composed of dissimilar metals and an effective |χ(3)|1020m2/V2 for either similar or dissimilar metals, increasing exponentially for smaller gaps. Field localization inside the gap ensures that harmonic generation arising from the gap region overwhelms intrinsic metal second- and third-order nonlinearities.

© 2014 Optical Society of America

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