For what is the first time, to our knowledge, we report on the extension of spectroscopic rotating-analyzer ellipsometry to generalized ellipsometry to define and to determine three essentially normalized elements of the optical Jones matrix J [ R. M. A. Azzam N. M. Bashara , J. Opt. Soc. Am.62, 1521 ( 1972)]. These elements are measured in reflection over the spectral range of 3.5–4.5 eV on different surface orientations of uniaxial TiO2 cut from the same bulk crystal. With a wavelength-by-wavelength regression and a 4 × 4 generalized matrix algebra, both refractive and absorption indices for the ordinary and the extraordinary waves, no, ko, ne, and ke, are determined. The inclinations and the azimuths of the optic axes with respect to the sample normal and plane of incidence were determined as well. The latter are confirmed by x-ray diffraction and polarization microscopy. Hence the spectrally dependent dielectric function tensor in laboratory coordinates is obtained. Very good agreement between measured and calculated data for the normalized Jones elements for the respective sample orientations and positions are presented. This technique may become an important tool for investigating layered systems with nonscalar dielectric susceptibilities.
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