Abstract: The invention provides new types of plasmon-driven growth mechanism for silver nanostructures involving the fusion of triangular nanoprisms. This mechanism, which is plasmon excitation-driven and highly cooperative, produces bimodal particle size distributions. In these methods, the growth process can be selectively switched between bimodal and unimodal distributions using dual beam illumination of the nanoparticles. This type of cooperative photo-control over nanostructure growth enables synthesis of monodisperse nanoprisms with a preselected edge length in the 30–120 nm range simply by using one beam to turn off bimodal growth and the other (varied over the 450–700 nm range) for controlling particle size.