We report on the evolution of the polaron and phonon mode properties in amorphous tungsten oxide thin films measured by spectroscopic ellipsometry in the infrared to ultraviolet spectral regions as a function of the intercalated proton density. A parametric physical model dielectric function is presented, which excellently describes the ellipsometry data over a large intercalated charge-density range. Upon increased amounts of intercalated charge we observe a strong increase in the polaron absorption in the visible spectral range, a decrease in the infrared W-O bond polarity, and an increase in the W=O bond polarity. Our findings support the oxygen-extraction model as the polaron formation mechanism in tungsten oxide in agreement with previous theoretical works based on first-principles pseudopotential calculations. We discuss and suggest polaron formation by oxygen-related defect generation as origin for the coloration mechanism in tungsten oxide. We further discuss possible evidence for very large effective mass of the polarons within the insulator-to-metal transition regime.
|Original language||English (US)|
|Journal||Physical Review B - Condensed Matter and Materials Physics|
|State||Published - Dec 1 2008|
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics