Symmetry-breaking synthetic controls allow for nanostructure geometries that are counter to the underlying crystal symmetry of a material. If suitably applied, such controls provide the means to drive an isotropic metal along a growth pathway yielding a three-dimensional chiral geometry. Herein, we present a light-driven solution-based synthesis yielding helical gold spirals from substrate-bound seeds. The devised growth mode relies on three separate symmetry-breaking events ushered in by seeds lined with planar defects, a capping agent that severely frustrates early stage growth, and the Coulombic repulsion that occurs when identically charged growth fronts collide. Together they combine to advance a growth pathway in which planar growth emanates from one side of the seed, advances to encircle the seed from both clockwise and counterclockwise directions, and then, upon collision of the two growth fronts, sees one front rise above the other to realize a self-perpetuating three-dimensional spiral structure.

Microsphere Photolithography (MPL) is a nanopatterning technique that utilizes a selfassembled monolayer of microspheres as an optical element to focus incident radiation inside a layer of photoresist. A Mie resonance in the microspheres produces a sub-diffraction limited photonic-jet on the opposite side of each microsphere from the illumination. When combined with pattern transfer techniques such as etching/lift-off, MPL provides a versatile, low-cost fabrication method for producing hexagonal close-packed metasurfaces. This paper investigates the MPL process for creating refractive index (RI) sensors on the cleaved tips of optical fiber. The resonant wavelength of metal elements on the surface is dependent on the local dielectric environment and allows the refractive index of an analyte to be resolved spectrometricly. A numerical study of hole arrays defined in metal films shows that the waveguide mode provides good sensitivity to the analyte refractive index. This can be readily tuned by adjusting the MPL exposure and the simulation results guide the fabrication of a defect tolerant refractive index sensor on the tip of a fiber tip with a sensitivity of 613 nm/RIU. The conformal nature of the microsphere monolayer simplifies the fabrication process and provides a viable alternative to direct-write techniques such as Focused Ion Beam (FIB) milling.

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Microsphere photolithography (MPL) is a fabrication technique that combines the ability to self-assemble arrays of microspheres with the ability of a microsphere to focus light to a photonic jet, in order to create highly ordered nanoscale features in photoresist. This paper presents a model of photoresist exposure with the photonic jet, combining a full-wave electromagnetic model of the microsphere/photoresist interaction with the sequential removal of exposed photoresist by the developer. The model is used to predict the dose curves for the MPL process based on the photoresist thickness, illumination conditions, and development time. After experimental validation, the model provides insight into the process including the resolution, sensitivity, and effects of off-normal illumination. This guides the fabrication of sub-100 nm hole/disk arrays using lift-off, and superposition is shown to predict the geometry for split-ring resonators created using multiple exposures. This model will assist synthesizing fabrication parameters to create large area scalable metasurfaces with sensing and energy management applications.

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