Electrically Tunable Harmonic Generation of Light from Plasmonic Structures in Electrolytes

An emerging trend in plasmonics is to exploit nanostructured metals as a self-contained electrooptic platform with simultaneously supported electrical and optical functions. When it comes to nonlinear optics, this dual electrical and optical functionality offers an exciting potential to enable electrically controlled wave mixing processes in various nanometallic systems. Here we demonstrate tunable nonlinear generation of light enabled by an electrically active plasmonic crystal in aqueous electrolytic solutions. A modulation depth of ∼150%/V is observed in the second-harmonic signal, thanks to the light concentrating ability of the resonant plasmonic structure as well as the voltage-assisted charge accumulation on the metallic surfaces. The hybrid plasmonic-electrolyte system demonstrated in this work offers the exciting new potential to use plasmonic nanostructures for voltage-controlled nonlinear signal generation and in situ biochemical sensing in an aqueous environment.