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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. [ABSTRACT FROM AUTHOR]

Absorption losses and laser-induced damage threshold (LIDT) are considered to be the major constraints for development of optical coatings for high-power laser optics. Such coatings require paramount properties, such as low losses due to optical absorption, high mechanical stability, and enhanced damage resistance, to withstand high-intensity laser pulses. In this work, heterostructures were developed by sub-nanometer thin films of SiO2 and HfO2 using the plasma-enhanced atomic layer deposition (PEALD) technique. Thin-film characterization techniques, such as spectroscopic ellipsometry, spectrophotometry, substrate curvature measurements, X-ray reflectivity, and Fourier transform infrared spectroscopy, were employed for extracting optical constants, residual stress, layer formation, and functional groups present in the heterostructures, respectively. These heterostructures demonstrate tunable refractive index, bandgap, and improved optical losses and LIDT properties. The films were incorporated into antireflection coatings (multilayer stacks and graded-index coatings) and the LIDT was determined at 355 nm wavelength by the R-on-1 method. Optical absorptions at the reported wavelengths were characterized using photothermal common-path interferometry and laser-induced deflection techniques. [ABSTRACT FROM AUTHOR]

The structural, optical, and mechanical properties of TiO2 nanolaminate films grown by plasma-enhanced atomic layer deposition are discussed. Several TiO2/Al2O3 and TiO2/SiO2 compositions have been investigated to study the effect of the relative number of ALD oxide cycles on the film properties to obtain a high refractive index coating with low optical losses, low roughness, and low mechanical stress. The formation of crystalline TiO2 observed at high deposition temperature, or film thickness was inhibited by periodically introducing ultra-thin amorphous layers into the film. Only 4 ALD cycles of Al2O3 (corresponding to ca. 0.5 nm) between 335 ALD cycles of TiO2 (ca. 11 nm) form a closed, distinct layer suppressing the crystallization in TiO2 film. Consequently, the roughness of the pure TiO2 film is reduced from ca. 20 nm rms to 1 nm rms in the 335/4 nanolaminate, with only a slight decrease of the refractive index from 2.46 to 2.44 in 100 nm pure TiO2 and the nanolaminate, respectively. The refractive indices of the nanolaminates in various compositions vary between 2.38 and 2.50 at 632 nm, and the corresponding optical losses from the films are low. The mechanical stress was reduced to about 140 MPa in several TiO2/Al2O3 nanolaminates; however, lower mechanical stress has not been obtained with the studied compositions. The nanolaminate structure is preserved up to 600 °C annealing temperature. After annealing at 800 °C, the individual layers interdiffuse into each other so that no distinct nanolaminate structure is detected. By using TiO2/Al2O3 nanolaminates with reduced mechanical stress, a narrow bandpass filter was realized on various substrates, including half-ball and aspherical lenses. [ABSTRACT FROM AUTHOR]

Ultra-thin metallic films are widely applied in optics and microelectronics. However, their properties differ significantly from the bulk material and depend on the substrate material. The nucleation, film growth, and layer properties of atomic layer deposited (ALD) iridium thin films are evaluated on silicon wafers, BK7, fused silica, SiO2, TiO2, Ta2O5, Al2O3, HfO2, Ru, Cr, Mo, and graphite to understand the influence of various substrate materials. This comprehensive study was carried out using scanning electron and atomic force microscopy, X-ray reflectivity and diffraction, four-point probe resistivity and contact angle measurements, tape tests, and Auger electron spectroscopy. Within few ALD cycles, iridium islands occur on all substrates. Nevertheless, their size, shape, and distribution depend on the substrate. Ultra-thin (almost) closed Ir layers grow on a Ta2O5 seed layer after 100 cycles corresponding to about 5 nm film thickness. In contrast, the growth on Al2O3 and HfO2 is strongly inhibited. The iridium growth on silicon wafers is overall linear. On BK7, fused silica, SiO2, TiO2, Ta2O5, Ru, Cr, and graphite, three different growth regimes are distinguishable. The surface free energy of the substrates correlates with their iridium nucleation delay. Our work, therefore, demonstrates that substrates can significantly tailor the properties of ultra-thin films. [ABSTRACT FROM AUTHOR]

[Display omitted] • Fabrication of ultrathin heterostructures of Al 2 O 3 /TiO 2 by atomic layer deposition. • Blue shift in optical bandgap indicates presence of quantizing effect. • Designing new materials with tunable refractive index and bandgap combinations. Atomically thin heterostructures and superlattices are promising candidates for various optoelectronic and photonic applications. Different combinations of Al 2 O 3 /TiO 2 composites are obtained by plasma enhanced atomic layer deposition (PEALD). Their growth, composition, dispersion relation, and optical bandgap are systematically studied by means of UV/VIS spectrophotometry, spectroscopic ellipsometry (SE), x-ray reflectometry (XRR), scanning transmission electron microscopy (STEM) and x-ray photoelectron spectroscopy (XPS). Besides, an effective medium approximation (EMA) approach is applied to model the heterostructures theoretically. The refractive index and the indirect bandgap of the heterostructures depend on the ratio of the two oxides, while the bandgap is very sensitive to the thicknesses of the barrier and quantum well layers. A large blue shift of the absorption edge from 400 nm to 320 nm is obtained by changing the TiO 2 (quantum well) thickness from ~2 nm to ~0.1 nm separated by ~2 nm of Al 2 O 3 (barrier) layers. PEALD unfolds the possibility of achieving optical quantizing effects within complex heterostructures enabling control of their structures down to atomic scale. It enables a path towards atomic scale processing of new 'artificial' materials with desired refractive indices and bandgap combinations by precise control of their compositions. [ABSTRACT FROM AUTHOR]