Plasmonic heterostructures are deterministically constructed in organized arrays through chemical pattern directed assembly, a combination of top-down litho graphy and bottom-up assembly, and by the sequential immobilization of gold nanoparticles of three different sizes onto chemically patterned surfaces using tailored interaction potentials. These spatially addressable plasmonic chain nanostructures demonstrate localization of linear and nonlinear optical fields as well as nonlinear circular dichroism.