Second- and third-harmonic generations for a nondilute suspension of coated particles with radial dielectric anisotropy

Abstract.

We derive expressions for the effective nonlinear susceptibility tensors for both the second harmonic generation (SHG) and induced third harmonic generation (THG) of nonlinear composite materials, in which nondilute coated particles with radial dielectric anisotropy are randomly embedded in the linear host. Two types of coated particles are considered. The first is that the core possesses a second order nonlinear susceptibility and the shell is linear and radially anisotropic, while the second is that the core is linear with radial anisotropy and the shell has a second order nonlinear susceptibility. We observe greatly enhanced SHG and THG susceptibilities at several surface plasmon resonant frequencies. For the second model, due to the coating material being metallic, there exists two fundamental resonant frequencies ω_c1 and ω_c2, whose difference ω_c2-ω_c1 is strongly dependent on the interfacial parameter and the radial dielectric anisotropy. Furthermore, in both systems, the adjustment of the dielectric anisotropy results in larger enhancement of both SHG and induced THG susceptibilities at surface plasmon resonant frequencies than the corresponding isotropic systems. Therefore, both the core-shell structure and the dielectric anisotropy play important roles in determining the nonlinear enhancement and the surface resonant frequencies.