Second-harmonic generation from spherical particles

We calculate the nonlinear dipole and quadrupole moments induced at the second-harmonic (SW) frequency 2 omega in a small dielectric sphere by an inhomogeneous monochromatic electric field of frequency omega. We neglect finite-size effects and assume that the selvedge region of the sphere is thin enough so that the surface may be considered locally flat. The second-order dipole displays resonances corresponding to the excitation of dipolar and quadrupolar plasmons at w and a dipolar plasmon at 2 omega, besides the resonances in the nonlinear surface response parameters a, b, and f. The second-order quadrupole, on the other hand, has resonances corresponding to those of a, b, and f, and to the excitation of dipolar surface plasmons at omega only. Depending on the relation between the size of the sphere and the spatial scale of variation of the field, the SH radiation may be dominated by either dipolar or quadrupolar scattering, with a crossover region. As an application, we calculate the SH scattering of a Si sphere lying at various distances above a dielectric substrate.