Harnessing collisional nonlinearity for enhanced harmonic generation by ultraviolet plasmonic nanoparticles

J Chem Phys. 2024 Aug 7;161(5):054111. doi: 10.1063/5.0210865.

Abstract

We investigate the contribution of inelastic electron collisions to nonlinear (NL) dynamics in ultraviolet plasmonic nanoparticles, exploring their potential for harmonic generation. Employing the Landau weak coupling formalism to model radiation-driven electron dynamics in sodium and aluminum, we account for both electron-electron and electron-phonon scattering processes by a set of hydrodynamic equations, which we solve perturbatively to obtain third-order NL susceptibilities. Furthermore, we model high harmonic generation enhanced by localized surface plasmons in nanospheres composed of such poor metals, demonstrating their efficient operation for extreme ultraviolet generation. Our investigation reveals that plasmonic nanospheres composed of sodium and aluminum produce a large field intensity enhancement of ≃103-105, boosting the harmonic generation process. Our findings indicate that poor metals hold great promise for advanced extreme ultraviolet nano-sources with potential applications in nano-spectroscopy.