Insights into nanoparticle shape transformation by energetic ions

Shape modification of embedded nanoparticles can be achieved by means of swift heavy ion irradiation. During irradiation, the particles elongate and align with the direction of the ion beam, presumably due to nanometer-scale phase transitions induced by individual ion impacts. However, the details of this transformation are not fully understood. The shape of metal nanoparticles embedded in dielectric matrices defines the non-linear optical properties of the composite material. Therefore, understanding the transformation process better is beneficial for producing materials with the desired optical properties. We study the elongation mechanism of gold nanoparticles using atomistic simulations. Here we focus on long-timescale processes and adhesion between the nanoparticle and the matrix. Without the necessity of ad-hoc assumptions used earlier, our simulations show that, due to adhesion with the oxide, the nanoparticles can grow in aspect ratio while in the molten state even after silicon dioxide solidifies. Moreover, they demonstrate the active role of the matrix: Only explicit simulations of ion impacts around the embedded nanoparticle provide the mechanism for continuous elongation up to experimental values of aspect ratio. Experimental transmission electron microscopy micrographs of nanoparticles after high-fluence irradiation support the simulations. The elongated nanoparticles in experiments and their interface structures with silica, as characterized by the micrographs, are consistent with the simulations. These findings bring ion beam technology forward as a precise tool for shaping embedded nanostructures for various optical applications