Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures

Abstract

The nonlinear refractive index of plasmonic materials may be used to obtain nonlinear functionality, e.g., power-dependent switching. Here, we investigate the nonlinear refractive index of single-crystalline gold in thin layers and nanostructures on dielectric substrates. In a first step, we implement a z-scan setup to investigate ~100-µm-sized thin-film samples. We determine the nonlinear refractive index of fused silica, n2(SiO2) = 2.9 × 10−20 m2/W, in agreement with literature values. Subsequent z-scan measurements of single-crystalline gold films reveal a damage threshold of 0.22 TW/cm2 and approximate upper limits of the real and imaginary parts of the nonlinear refractive index, |n2′(Au)| < 1.2 × 10−16 m2/W and |n2″(Au)| < 0.6 × 10−16 m2/W, respectively. To further determine possible effects of a nonlinear refractive index in plasmonic circuitry, interferometry is proposed as a phase-sensitive probe. In corresponding nanostructures, relative phase changes between two propagating near-field modes are converted to amplitude changes by mode interference. Power-dependent experiments using sub-10-fs near-infrared pulses and diffraction-limited resolution (NA = 1.4) reveal linear behavior up to the damage threshold (0.23 times relative to that of a solid single-crystalline gold film). An upper limit for the nonlinear power-dependent phase change between two propagating near-field modes is determined to Δφ < 0.07 rad.