This paper presents a spectroscopic study using the techniques of ellipsometry and infrared (IR) absorption spectroscopy of the chemical bonding in silicon dioxide (SiO2) films grown in dry oxygen ambients at temperatures between 550 and 1000 °C. We find that the index of refraction at 632.8 nm increases and the frequency of the dominant IR active bond-stretching vibration at about 1075 cm−1 decreases as the growth temperature is decreased below 1000 °C. Comparing the properties of these films with suboxides (SiOx, x<2) grown by plasma-enhanced chemical vapor deposition, and compacted bulk silica has lead us to conclude: (i) that films grown at temperatures at or below 1000 °C are homogeneous stoichiometric oxides (SiO2); and (ii) that the systematic and correlated variations in the index of refraction and the IR frequency result from increases in the film density with decreasing growth temperature. We present a microscopic model that accounts for (i) the increases in the density and the index of refraction; and (ii) the accompanying decrease in the IR stretching frequency in terms of a decrease in the Si–O–Si bond angle.