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The structural symmetry of solids plays an important role in defining theirlinear and nonlinear optical properties. The quest for versatile,cost-effective, large-scale, and defect-free approaches and materials platformsfor tailoring structural and optical properties on demand has been underway fordecades. We experimentally demonstrate a bottom-up self-assembly-based organicengineered material comprised of synthesized molecules with large dipolemoments that are crystallized into a spherulite structure. The molecules alignin an azimuthal direction, resulting in a vortex polarity with spontaneouslybroken symmetry leading to strong optical anisotropy and nonlinear opticalresponses. These unique polarization properties of the judiciously designedorganic spherulite combined with the symmetry of structured optical beamsenable a plethora of new linear and nonlinear light-matter interactions,including the generation of optical vortex beams with complex spin states andon-demand topological charges at the fundamental, doubled, and tripledfrequencies. The results of this work are likely to enable numerousapplications in areas such as high-dimensional quantum information processing,with large capacity and high security. The demonstrated spherulite crystalsfacilitate stand-alone micro-scale devices that rely on the unique micro-scalespontaneous vortex polarity that is likely to enable future applications forhigh-dimensional quantum information processing, spatiotemporal opticalvortices, and a novel platform for optical manipulation and trapping.

Optical vortices enabled by structural vortices