Plasmon enhanced second harmonic generation by periodic arrays of triangular nanoholes coupled to quantum emitters

Abstract

Optical properties of periodic arrays of nanoholes of a triangular shape with experimentally realizable parameters are examined in both linear and nonlinear regimes. Utilizing fully vectorial three-dimensional approach based on the nonlinear hydrodynamic Drude model describing metal coupled to Maxwells equations and Bloch equations for molecular emitters we analyze linear transmission, reflection, and nonlinear power spectra. Rigorous numerical calculations demonstrating second and third harmonic generation by the triangular hole arrays are performed. It is shown that both the Coulomb interaction of conduction electrons and the convective term contribute on equal footing to the nonlinear response of metal. It is demonstrated that the energy conversion efficiency in the second harmonic process is the highest when the system is pumped at the localized surface plasmon resonance. When molecular emitters are placed on a surface of the hole array lineshapes of the second harmonic signal exhibits three peaks corresponding to second harmonics of the localized surface plasmon mode and upper and lower polaritonic states.