We describe a novel ion-implantation method for fabricating a dichroic nanoparticle film by controlling the nucleation and growth of silver nanoparticles in fused silica. We first implant Sc and O ions into the silica substrate to create a high-index layer and modify the shortand intermediate-range order; this dual-implantation technique defines a sharper interface between the silica substrate and the nanoparticle layer. By modifying the shortand intermediate-range order in a thin layer of the silica matrix, Ag ions that are subsequently implanted are subject to altered diffusion and nucleation dynamics, yielding a bilayer structure comprising spatially separated regions of smaller and larger Ag nanoparticles. Depending on the implanted dose of Sc, the peak resonant wavelength in reflectivity can shift as much as 100 nm between front-side (implanted face) and back-side (non-implanted face) illumination. Implications for the optimization of bidirectional optical filters and optical cavities are discussed and compared to calculations of scattering efficiency based on Mie theory.