Multispectral Holographic Intensity and Phase Imaging of Semitransparent Ultrathin Films.

In this paper, we demonstrate a novel optical characterization method for ultrathin semitransparent and absorbing materials through multispectral intensity and phase imaging. The method is based on a lateral-shearing interferometric microscopy (LIM) technique, where phase-shifting allows extraction of both the intensity and the phase of transmitted optical fields. To demonstrate the performance in characterizing semitransparent thin films, we fabricated and measured cupric oxide (CuO) seeded gold ultrathin metal films (UTMFs) with mass-equivalent thicknesses from 2 to 27 nm on fused silica substrates. The optical properties were modeled using multilayer thin film interference and a parametric model of their complex refractive indices. The UTMF samples were imaged in the spectral range from 475 to 750 nm using the proposed LIM technique, and the model parameters were fitted to the measured data in order to determine the respective complex refractive indices for varying thicknesses. Overall, by using the combined intensity and phase not only for imaging and quality control but also for determining the material properties, such as complex refractive indices, this technique demonstrates a high potential for the characterization of the optical properties, of (semi-) transparent thin films.

Transverse Hypercrystals Formed by Periodically Modulated Phonon Polaritons.

Photonic crystals and metamaterials are two overarching paradigms for manipulating light. By combining these approaches, hypercrystals can be created, which are hyperbolic dispersion metamaterials that undergo periodic modulation and mix photonic-crystal-like aspects with hyperbolic dispersion physics. Despite several attempts, there has been limited experimental realization of hypercrystals due to technical and design constraints. In this work, hypercrystals with nanoscale lattice constants ranging from 25 to 160 nm were created. The Bloch modes of these crystals were then measured directly using scattering near-field microscopy. The dispersion of the Bloch modes was extracted from the frequency dependence of the Bloch modes, revealing a clear switch from positive to negative group velocity. Furthermore, spectral features specific to hypercrystals were observed in the form of sharp density of states peaks, which are a result of intermodal coupling and should not appear in ordinary polaritonic crystals with an equivalent geometry. These findings are in agreement with theoretical predictions that even simple lattices can exhibit a rich hypercrystal bandstructure. This work is of both fundamental and practical interest, providing insight into nanoscale light-matter interactions and the potential to manipulate the optical density of states.

Tuning of Ultra-Thin Gold Films by Photoreduction.

Ultrathin metal films (UTMFs) are used in a wide range of applications, from transparent electrodes to infrared mirrors and metasurfaces. Due to their small thickness (<5 nm), the electrical and optical properties of UTMFs can be changed by external stimuli, for example, by applying an electric field through an ion gel. It is also known that oxidized thin films and nanostructures of Au can be reduced by irradiating with short-wavelength light. Here we show that the resistance, reflectance, and resonant optical response of Au UTMFs is changed significantly by ultraviolet light. More specifically, photoreduction and oxidation processes can be sequentially applied for continuous tuning, with observed modulation ranges for sheet resistance (Rs) and reflectance of more than 40% and 30%, respectively. The proposed method has the potential for achieving reconfigurable UTMF structures and trimming their response to specific working points, e.g., a predetermined resonance wavelength and amplitude. This is also important for large scale deployment of such surfaces as one can compensate material nonuniformity, morphological, and structural dimension errors occurring during fabrication.

Ultrathin Metals on a Transparent Seed and Application to Infrared Reflectors.

Ultrathin metal films (UTMFs) are widely used in optoelectronic applications, from transparent conductors to photovoltaic cells, low emissivity windows, and plasmonic metasurfaces. During the initial deposition phase, many metals tend to form islands on the receiving substrate rather than a physically connected (percolated) network, which eventually evolves into continuous films as the thickness increases. For example, in the case of Ag and Au on dielectric surfaces, percolation begins when the thickness of the metal film is at least about 5 nm. It is known that the type of growth can be changed when a proper seed layer is used. Here, we show that a CuO layer directly deposited on a substrate can dramatically influence surface wetting and promote early percolation of polycrystalline Ag and Au UTMFs. We demonstrate that the proposed seed is effective even when its thickness is sub-nanometric, in this way maintaining the full transparency of the receiving substrate. The Ag and Au films seeded with CuO showed a percolation thickness close to 1 nm and were morphologically and optically characterized from an ultraviolet (λ = 300 nm) to a midinfrared (λ = 15 µm) wavelength. Infrared reflectors, a mirror and a resonant plasmonic structure, were also demonstrated and uniquely tuned by electrical gating, this being possible owing to the small thickness of the constituting Au UTMF.