Ultrafast All-optical Modulation Exploiting the Vibrational Dynamic of Metallic Meta-atoms

Abstract: Optical control over elementary molecular vibration establishes fundamental capabilities for exploiting the broad range of optical linear and nonlinear phenomena. However, experimental demonstration of the coherently driven molecular vibration remains a challenge task due to the weak optical force imposed on natural materials. Here we report the design of "meta-atom" that exhibits giant artificial optical nonlinearity. These "meta-atoms" support co-localized magnetic resonance at optical frequency and vibration resonance at GHz frequency with a deep-sub-diffraction-limit spatial confinement (${\lambda}^2/100$). The coherent coupling of those two distinct resonances manifests a strong optical force, which is fundamentally different from the commonly studied form of radiation forces, the gradient forces, or photo-thermal induced deformation. It results in a giant third-order susceptibility $\chi^{(3)}$ of $10^{-13}$ $m^2$/$V^2$, which is more than six orders of magnitude larger than that found in natural materials. The all-optical modulation at the frequency well above 1 GHz has thus been demonstrated experimentally.