Optical generation, templating, and polymerization of three-dimensional arrays of liquid-crystal defects decorated by plasmonic nanoparticles

Defects in liquid crystals are used to model topological entities ranging from Skyrmions in high-energy physics to early-universe cosmic strings, as well as find practical applications in self-assembly of diffraction gratings and in scaffolding of plasmonic nanoparticles, but they are hard to control and organize into three-dimensional lattices. We laterally scan focused laser beams to produce periodic arrays of twist-stabilized defects forming either linear (fingers) or axially symmetric (torons) configurations in partially polymerizable liquid crystal films. Polymerization allows for stabilization of these structures and the formation of three-dimensional arrays of defects by stacking of the thin cholesteric films on top of each other. In the process of fabrication of such arrays, we polymerize the liquid crystal film with an array of torons or fingers and then sequentially produce and photopolymerize new liquid crystal layers on top of it, thus obtaining a three-dimensional structure of twist-stabilized defects in a layer-by-layer fashion. Templating by the polymerized layer spontaneously yields ordered organization of fingers and torons in the new cholesteric layer, thus enabling a three-dimensional ordered structure of defects. Nondestructive three-dimensional imaging of director fields by use of three-photon excitation fluorescence polarizing microscopy reveals the nature of topological singularities and physical underpinnings behind the observed templating effect. Three-dimensional patterning of defects templates the self-assembly of plasmonic nanoparticles into individual singularities and their arrays, laying the groundwork for potential applications in nanophotonics, plasmonics, metamaterial fabrication, and nanoscale energy conversion.