Enhancement of the complex third-order nonlinear optical susceptibility in Au nanorods

We experimentally determined the dispersion of the complex third-order nonlinear optical susceptibility χ(3) of Au nanorods over a wide bandwidth (370 – 800 nm). Compared to bulk Au, these nanorods exhibit greatly enhanced nonlinearities that can be manipulated by geometrical parameters. Accurately measuring the χ(3) values of nanostructured metals is challenging because χ(3) is strongly influenced by the local field effects. Hence the current published χ(3) values for Au nanorods have huge variations in both magnitude and sign because Z-scan measurements are used almost exclusively. This work combines pump-probe methods with spectroscopic ellipsometry to show that Au nanorods exhibit strong wavelength dependence and enhanced χ(3) in the vicinity of the longitudinal plasmon mode and explains where the regions of SA and RSA exist and how focusing and defocusing affects χ(3). In this context, the results highlight the importance of the dispersion of the quantity χ(3) to design plasmonic platforms for nanophotonics applications.