The optical properties of cascaded plasmon resonant metallic nanocomposites are investigated. Plasmon resonances and their related field distributions are numerically evaluated in two-dimensional arrays of spherical silver nanoparticles embedded in a dielectric host. The field distributions in structures with identical particle sizes indicate the presence of a largely dipolar particle response, with a small multipole resonance contribution at high frequency. However, in arrays consisting of particles with dissimilar sizes, an additional coupled mode appears in which the dipole moment in adjacent particles is found to be anti-parallel. For increasing size-dissimilarity a higher electric field enhancement is observed inside the small metal nanospheres, indicative of a cascaded field enhancement effect. This effect may be used to enhance the nonlinear optical response of an effective medium composed of particles with engineered size dispersion and particle placement.© (2011) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.