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In this article, we develop a classical electrodynamic theory to study the optical nonlinearities of metallic nanoparticles. The quasi-free electrons inside the metal are approximated as a classical Coulomb-interacting electron gas, and their motion under the excitation of an external electromagnetic field is described by the plasma equations. This theory is further tailored to study second-harmonic generation. Through detailed experiment-theory comparisons, we validate this classical theory as well as the associated numerical algorithm. It is demonstrated that our theory not only provides qualitative agreement with experiments, it also reproduces the overall strength of the experimentally observed second-harmonic signals.
Strong second-harmonic generation has recently been experimentally observed from metamaterials consisting of periodic arrays of metal split ring resonators with an effective negative magnetic permeability [Science, 313, 502 (2006)]. To explore the un
The resonance effects on the optical second harmonic generation from 140 nm silver nanoparticles is studied experimentally by hyper-Rayleigh scattering and numerically by finite element method calculations. We find that the interferences between the
On the basis of the Edward-Kornfeld formulation, we study the effective susceptibility of secondharmonic generation (SHG) in colloidal crystals, which are made of graded metallodielectric nanoparticles with an intrinsic SHG susceptibility suspended i
The generation process of second harmonic (SH) radiation from holes periodically arranged on a metal surface is investigated. Three main modulating factors affecting the optical response are identified: the near-field distribution at the wavelength o
We study second harmonic generation in nonlinear, GaAs gratings. We find large enhancement of conversion efficiency when the pump field excites the guided mode resonances of the grating. Under these circumstances the spectrum near the pump wavelength