Broadband Spin and Orbital Momentum Modulator Using Self‐Assembled Nanostructures

Abstract The structural symmetry of solids plays an important role in defining their linear and nonlinear optical properties. The quest for versatile, cost‐effective, large‐scale, and defect‐free approaches and materials platforms for tailoring structural and optical properties on demand is underway since decades. A self‐assembled spherulite material comprised of synthesized molecules with large dipole moments aligned azimuthally, forming a vortex polarity with spontaneously broken symmetry, is experimentally demonstrated. This unique self‐assembled structure enables new linear and nonlinear light–matter interactions, including generating optical vortex beams with complex spin states and on‐demand topological charges at the fundamental, doubled, and tripled frequencies. This work will likely enable numerous applications in areas such as high‐dimensional quantum information processing with large capacity and high security, spatiotemporal optical vortices, and a novel optical manipulation and trapping platform.