In 1950, a quarter of a century after his first-ever nonlinear optical experiment when intensity-dependent absorption was observed in uranium-doped glass, Sergey Vavilov predicted that birefringence, dichroism and polarization rotatory power should be dependent on light intensity. It required the invention of the laser to observe the barely detectable effect of light intensity on the polarization rotatory power of the optically active lithium iodate crystal, the phenomenon now known as the nonlinear optical activity, a high-intensity counterpart of the fundamental optical effect of polarization rotation in chiral media. Here we report that a plasmonic metamaterial exhibits nonlinear optical activity 30 million times stronger than lithium iodate crystals, thus transforming this fundamental phenomenon of polarization nonlinear optics from an esoteric phenomenon into a major effect of nonlinear plasmonics with potential for practical applications.

Periodic nanostructuring can enhance the optical nonlinearity of plasmonic metals by several orders of magnitude. By patterning a gold film, the largest sub-100 femtosecond nonlinearity is achieved, which is suitable for terahertz rate all-optical data processing as well as ultrafast optical limiters and saturable absorbers.

Plasmonic metasurfaces have recently attracted much attention because of their novel characteristics with respect to light polarization and wave front control on deep-subwavelength scales. The development of metasurfaces with reconfigurable optical responses is opening new opportunities in high-capacity communications, real-time holograms and adaptive optics. Such tunable devices have been developed in the mid-infrared spectral range and operated in light intensity modulation schemes. Here we present a novel optically reconfigurable hybrid metasurface that enables polarization tuning at optical frequencies. The functionality of tuning is realized by switching the coupling conditions between the plasmonic modes and the binary isomeric states of an ethyl red switching layer upon light stimulation. We achieved more than 20° nonlinear changes in the transmitted polarization azimuth using just 4 mW of switching light power. Such design schemes and principles could be easily applied to dynamically adjust the functionalities of other metasurfaces.