Optical and plasmonic properties of high electron density epitaxial and oxidative controlled titanium nitride thin films

Abstract: This work reports a pulsed laser-assisted synthesis, detailed structural characterization, and study of plasmonic properties of three sets of TiN/TiNO thin films with high electron density. The first two sets of TiN films were grown at 600C and 700C under a high vacuum condition. The third set of TiN film was grown in the presence of 5 mTorr of molecular oxygen at 700C. The results have shown that TiN films deposited in a high vacuum are metallic, have large optical reflectance, and have high optical and electrical conductivity. The TiN films, grown in 5 mTorr O2, were partially oxidized and semiconducting with room temperature resistivity nearly three times larger than those of the TiN films grown under high vacuum conditions. The optical conductivity of these films was analyzed using a Kramers-Kronig transformation of reflectance and a Lorentz-Drude model; the optical conductivity determined by these two different methods agreed very well. To corroborate our experimental spectral observations, we have calculated the phonon dispersions and Raman active modes of TiNO using the virtual crystal approximation. A comparative analysis of the phonon dispersions between rutile TiO2 and rocksalt TiNO has shown that the incorporation of nitrogen atoms does not significantly alter the phonon dispersions of rutile TiO2. However, it results in the emergence of new phonon modes at approximately 7.128 THz at the Gamma point, which corresponds to the experimentally observed Multi-Photon Phase-MPP. From the collateral study of experimental results and theoretical corroboration, a suitable multi-layer optical model was proposed for the TiN/TINO epitaxial thin films to extract the individual complex dielectric function from which many other optical parameters can be calculated.