The formation mechanism and step‐coverage quality of SiO2 films formed by the pyrolysis of tetraethylorthosilicate (TEOS) were studied, using a novel experimental technique called the “multi‐layered micro/macrocavity method.” The growth rate profiles at millimeter (macrocavity) and submicron (microtrench) sales deposited under a total pressure ranging from 2 to 760 Torr were simultaneously analyzed. The step coverage approaches conformal deposition either with decreasing volume‐to‐surface ratio (V/S) of the macrocavity reaction zone or with increasing total pressure. Combining these results with the growth‐rate profiles of the macrocavity shows that two kinds of intermediate species participate in deposition. One is a high‐activity species with a surface sticking probability near 1, and the other is a low‐activity. A nonlinear increase of the growth rate with the macrocavity V/S ratio indicates that a polymerization reaction occurs in the gas phase. A comprehensive model of the deposition kinetics is presented to correlate the step coverage quality and the growth rate uniformity with the operating conditions.

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