Broadband Spin and Orbital Momentum Modulator Using Self-Assembled Nanostructures.

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.