Control over particle structure in the radial direction. (A) Schematic of a fiber containing a cylindrical core consisting of nested shells undergoes the PRI-driven breakup into spherical multilayer particles. The cladding is not shown for clarity. (B) SEM micrograph of a three-layer core sectioned using a focused ion beam (FIB) with the PRI arrested before complete breakup of the core (G, As2S3; and P, PES). (C and D) Optical transmission micrographs of five-layer particles after breakup held in the polymer (P) cladding separated by smaller multilayered satellite particles. (E–H) Optical reflection micrographs of fiber multilayered-core cross-sections (G, As2S3; and P, PES). Schematics of the fiber structures are also shown. (I–L) SEM micrographs of multilayer particles after sectioning with a raster-scanning low-current FIB. Schematic of the particles are shown above each panel. G1, As2S3; G2, Ge1.3(As2Se3)98.7; P, PES.