Nonlocality-driven supercontinuum white light generation in plasmonic nanostructures

Structured plasmonic metals are widely employed for achieving nonlinear functionalities at the nanoscale due to their ability to confine and enhance electromagnetic fields and strong, inherent nonlinearity. Optical nonlinearities in centrosymmetric metals are dominated by conduction electron dynamics, which at the nanoscale can be significantly affected by the nonlocal effects. Here we show that nonlocal corrections, being usually small in the linear optical response, define nonlinear properties of plasmonic nanostructures. Using a full non-perturbative time-domain hydrodynamic description of electron plasma under femtosecond excitation, we numerically investigate harmonic generation in metallic Archimedean nanospirals, revealing the interplay between geometric and nonlocal effects. The quantum pressure term in the nonlinear hydrodynamic model results in the emergence of fractional nonlinear harmonics leading to broadband coherent white-light generation. The described effects present a novel class of nonlinear phenomena in metallic nanostructures determined by nonlocality of the electron response. A theoretical description of the nonlinear response of metals is complicated due to their complex electron behavior. Here, Krasavin et al . use a hydrodynamic model coupled with Maxwell's equations and demonstrate higher harmonics and supercontinuum generation from metal Archimedean spiral shapes