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10 May 2010 Effective medium multipolar tensor analysis of second-harmonic generation from metal nanoparticles
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Second-order nonlinear optical effects are electric-dipole-forbidden in centrosymmetric materials, but become allowed through magnetic-dipole and electric-quadrupole effects. Furthermore, such higher multipole effects can play a role also in the response of non-centrosymmetric materials, as demonstrated for second-harmonic generation (SHG) from chiral thin films of organic molecules and from metal nanostructures. For nanostructured materials, higher multipole effects can occur due to elementary light-matter interactions or due to field retardation across nanoparticles. For SHG from metal nanostructures, the latter mechanism was operative and associated with nanoscale defects, which attract strong local fields. The evidence of multipolar SHG emission was obtained from the different radiative properties of the various multipolar sources. The goal of the present work is to perform a more comprehensive multipolar analysis of SHG from arrays of L-shaped metal nanoparticles. In particular, we seek evidence of the presence of multipole interactions also at the fundamental frequency by performing detailed polarization measurements of the SHG response and relying on the different transformation properties of the various multipolar interactions for SHG emitted in the transmitted and reflected directions and for the fundamental beam incident on the metal or substrate side of the sample.
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Mariusz Zdanowicz, Sami Kujala, Hannu Husu, and Martti Kauranen "Effective medium multipolar tensor analysis of second-harmonic generation from metal nanoparticles", Proc. SPIE 7712, Nanophotonics III, 77121O (10 May 2010);

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