We studied the nonlinear optical response of metallic amorphous composite layers in terms of a self-phase-modulated, third-order Kerr nonlinearity. A nonlinear effective medium theory was used to describe low densities of gold and iridium nanoparticles embedded in an equally nonlinear host material. The fill fraction strongly influences the effective nonlinear susceptibility of the materials, increasing it by orders of magnitude in the case of gold due to localized surface plasmonic resonances. The enhancement of the nonlinear strength in amorphous composites with respect to the bulk material has an upper limit in metallic composites as dominating absorption effects take over at higher fill factors. Both saturated and induced absorption in the thin films of amorphous composites were observed depending on the selected frequency and relative position to the resonant frequency of electron excitation in the metallic inclusions. We demonstrated the depths to which thin films are affected by nonlinear enhancement effects.

Nonlinear optical phenomena enable novel photonic and optoelectronic applications. Especially, metallic nanoparticles and thin films with nonlinear optical properties offer the potential for micro-optical system integration. For this purpose, new nonlinear materials need to be continuously identified, investigated, and utilized for nonlinear optical applications. While noble-metal nanoparticles, nanostructures, and thin films of silver and gold have been widely studied, iridium (Ir) nanoparticles and ultrathin films have not been investigated for nonlinear optical applications yet. Here, we present a combined theoretical and experimental study on the linear and nonlinear optical properties of iridium nanoparticles deposited via atomic layer deposition (ALD). Linear optical constants, such as the effective refractive index and extinction coefficient, were evaluated at different growth stages of nanoparticle formation. Both linear and nonlinear optical properties of these Ir ALD coatings were calculated theoretically using the Maxwell Garnett theory. The third-order susceptibility of iridium nanoparticle samples was experimentally investigated using the z-scan technique. According to the experiment, for an Ir ALD coating with 45 cycles resulting in iridium nanoparticles, the experimentally determined nonlinear third-order susceptibility is about χIr(3) = (2.4 − i2.1) × 10−17 m2/V2 at the fundamental wavelength of 700 nm. The theory fitted to the experimental results predicts a 5 × 106-fold increase around 230 nm. This strong increase is due to the proximity to the Mie resonance of iridium nanoparticles.