Nature Mater. http://dx.doi.org/10.1038/nmat3148 (2011)

Phase conjugation implemented via a thin nonlinear film has been proposed as an alternative to the use of lossy, narrowband and complex metamaterials for realizing the phenomenon of negative refraction, albeit at microwave frequencies. Stefano Palomba and colleagues from the USA, the UK and Israel have now demonstrated a simpler solution that operates at optical frequencies by exploiting degenerate four-wave mixing (FWM) in a 20-nm-thick nanostructured gold film. They experimentally demonstrated that a beam generated during the FWM process can emerge at a negative angle relative to the exciting wave. Mixing two plane waves at frequency ω1 and incidence angle θ1 with a third plane wave at frequency ω2 and incidence angle θ2 gives rise to two beams at a new frequency of ω3 = 2ω1ω2 and incidence angle θ3 in the forwards and backwards directions. The intriguing phenomenon occurs for θ1 = 0, where the forwards nonlinear FWM beam exhibits negative refraction relative to the probe beam. The ratio between the sines of the incidence and refracted angles is a constant that depends only on the two wavelengths, which implies that the refractive index can be modified simply by tuning the wavelengths of the interacting waves. The team have experimentally shown that FWM for Au/SiO2/Au nanodisk metamaterials is around ten times stronger than that for smooth gold film, owing to the strong field confinement at localized surface plasmon resonances. They also obtained FWM efficiencies of 9 × 10−8 for a smooth gold film and 10−6 for nanodisk metamaterials. The findings are potentially useful for high-resolution and background-free imaging at the nanoscale.