Optically Governed Dynamic Surface Charge Redistribution of Hybrid Plasmo‐Pyroelectric Nanosystems

Abstract Though plasmonic effect is making some headway in the energy harvesting realm, its fundamental charge transfer mechanism to a large extent is attributed to the hot‐carrier generation at the contact interface. Herein this work attempts to elucidate the physical origin of light induced plasmo‐pyroelectric enhancement based on charge density manipulation on surface state in the vicinity of the metal–ferroelectric contact interface. More importantly, by tuning the band bending, it is shown that the charge density on the surface state of a hybrid plasmo‐pyroelectric (BaTiO₃‐Ag) nanosystem can be manipulated and largely increased under the resonant blue light illumination (363 nm). It is also demonstrated that owing to this effect, the spatial pyroelectric activity of a hybrid plasmo‐pyroelectric nanosystem governs 46% enhancement in pyroelectric coefficient. This research highlights the optically regulated charge density in plasmo‐pyroelectric nanosystems, which could pave a new avenue for energy harvesting/conversion devices with distinguished advantages in wireless, photonic‐controlled, localized, and dynamic stimulation.