Taivo Jõgiaas

Coatings with tunable refractive index and high mechanical resilience are useful in optical systems. In this work, thin films of HfO2 doped with Al2O3 were deposited on silicon at 300 °C by using plasma-enhanced atomic layer deposition (PE-ALD). The mainly amorphous 60–80 nm thick films consisted Al in the range of 2 to 26 at. %. The refractive indexes varied from 1.69 to 2.08 at the wavelength of 632 nm, and they consistently depended on the composition. The differences were higher in the UV spectral region. At the same time, the hardness of the films was from 12–15 GPa; the modulus was in the range of 160–180 GPa; and the mechanical properties did not have a good correlation with the deposited compositions. The deposition conditions, element contents, and refractive indexes at respective wavelengths were correlated. The results indicated that it is possible to tune optical properties and retain mechanical properties of atomic layer-deposited thin films of HfO2 with Al2O3 as doping oxide. Such films could be used as mechanically resilient and optically tunable coatings in, for instance, micro- or nano-electromechanical systems or transparent displays.

Mechanical properties of thin films are significant for the applicability of nanodevices. Amorphous Al2O3-Ta2O5 double and triple layers were atomic layer-deposited to the thickness of 70 nm with constituent single-layer thicknesses varying from 40 to 23 nm. The sequence of layers was alternated and rapid thermal annealing (700 and 800 °C) was implemented on all deposited nanolaminates. Annealing caused changes in the microstructure of laminates dependent on their layered structure. Various shapes of crystalline grains of orthorhombic Ta2O5 were formed. Annealing at 800 °C resulted in hardening up to 16 GPa (~11 GPa prior to annealing) in double-layered laminate with top Ta2O5 and bottom Al2O3 layers, while the hardness of all other laminates remained below 15 GPa. The elastic modulus of annealed laminates depended on the sequence of layers and reached up to 169 GPa. The layered structure of the laminate had a significant influence on the mechanical behavior after annealing treatments.

SiO2 films were grown to thicknesses below 15 nm by ozone-assisted atomic layer deposition. The graphene was a chemical vapor deposited on copper foil and transferred wet-chemically to the SiO2 films. On the top of the graphene layer, either continuous HfO2 or SiO2 films were grown by plasma-assisted atomic layer deposition or by electron beam evaporation, respectively. Micro-Raman spectroscopy confirmed the integrity of the graphene after the deposition processes of both the HfO2 and SiO2. Stacked nanostructures with graphene layers intermediating the SiO2 and either the SiO2 or HfO2 insulator layers were devised as the resistive switching media between the top Ti and bottom TiN electrodes. The behavior of the devices was studied comparatively with and without graphene interlayers. The switching processes were attained in the devices supplied with graphene interlayers, whereas in the media consisting of the SiO2-HfO2 double layers only, the switching effect was not observed. In addition, the endurance characteristics were improved after the insertion of graphene between the wide band gap dielectric layers. Pre-annealing the Si/TiN/SiO2 substrates before transferring the graphene further improved the performance.