We experimentally demonstrate enhanced third-harmonic generation from indium tin oxide nanolayers at telecommunication wavelengths with an efficiency that is approximately 600 times larger than crystalline silicon (Si). The increased optical nonlinearity of the fabricated nanolayers is driven by their epsilon-near-zero response, which can be tailored on-demand in the near-infrared region. The present material platform is obtained without any specialized nanofabrication process and is fully compatible with the standard Si-planar technology. The proposed approach can lead to largely scalable and highly integrated optical nonlinearities in Si-integrated devices for information processing and optical sensing applications.

Deterministic Aperiodic (DA) arrays of gold (Au) nanoparticles are proposed as a novel approach for the engineering of reproducible surface enhanced Raman scattering (SERS) substrates. A set of DA and periodic arrays of cylindrical and triangular Au nanoparticles with diameters ranging between 50–110 nm and inter-particle separations between 25–100 nm were fabricated by e-beam lithography on quartz substrates. Using a molecular monolayer of pMA (p-mercaptoaniline) as a Raman reporter, we show that higher values of SERS enhancement factors can be achieved in DA structures compared to their periodic counterparts, and discuss the specific scaling rules of DA arrays with different morphologies. Electromagnetic field calculations based on the semi-analytical generalized Mie theory (GMT) fully support our findings and demonstrate the importance of morphology-dependent diffractive coupling (long-range interactions) for the engineering of the SERS response of DA arrays. Finally, we discuss optimization strategies based on the control of particles sizes and shapes, and we demonstrate that spatially-averaged SERS enhancement factors of the order of ~ 10⁷ can be reproducibly obtained using DA arrays of Au nano-triangles. The ability to rigorously design lithographically fabricated DA arrays of metal nanoparticles enables the optimization and control of highly localized plasmonic fields for a variety of chip-scale devices, such as more reproducible SERS substrates, label-free bio-sensors and non-linear elements for nano-plasmonics.

Alternative plasmonic materials have attracted considerable attention due to their advantages compared to conventional metals, including compatibility with Si processing, tunability of optical properties, and reduced losses. In this work, we demonstrate that post-deposition annealing of materials fabricated by magnetron sputtering allows large tuning of the structural and the optical dispersion properties of Indium Tin Oxide (ITO), Al-doped ZnO (AZO) and Titanium Nitride (TiN) nano-layers. By measuring their optical bandgaps, we show that thermal annealing treatments can dramatically modulate the carrier concentration in these materials, thus providing tunability of the optical losses and enabling the engineering of Epsilon-Near-Zero (ENZ) regime. Besides, we perform X-ray diffraction (XRD) measurements to show that thermal annealing can also effectively tune the materials grain sizes. Eventually, the effect of different annealing gases on the free carrier concentration has also been investigated. The wide tunability and control of the optical and structural properties that we demonstrated in this work is important to engineer resonant optical responses across a wide frequency spectrum for device applications to plasmonics, metamaterials and transformation-optics.