Quasicylindrical Waves for Ordered Nanostructuring

Laser-induced self-organization of periodic nanostructures on highly absorbing materials is widely understood to be due to interference between laser and surface plasmon polaritons (SPPs) that are excited by initial surface roughness. The structure order naturally emerges from the propagation phase of SPPs. Here, we reveal an unexplored mechanism that is predominantly induced by quasicylindrical waves (QCWs) with negligible contributions from SPPs. This mechanism features a new principle of order emergence in growth of periodic nanostructures through short-range electromagnetic interactions between QCWs and marginal nanofringes. In this scenario, the periodicity of nanostructures is not simply determined by the electromagnetic wavelength. With suppressed long-range interactions, the formation of nanostructures shows a domino-like growth process, thus significantly improving structure uniformity. An in situ microscopic observation is performed to characterize the temporal dynamics of structural growth and verify the new mechanism. Further, the QCWs are directly observed in experiments, which are theoretically supported by a scattering model.