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Thermodynamic studies of the Si‐H‐Cl system are widely available. The results of these studies vary due to differences in the number of gas‐phase components used and differences in the basic thermodynamic data employed. This work describes the first experimental study to determine the equilibrium Si/Cl ratio as a function of Cl/H and temperature. The experimental results fall near those which are calculated, though they do not uniquely support any one of the theoretical studies. Computational studies make the assumption that the Cl/H ratio is constant for the silicon CVD reaction. It is shown in this study that this is not always the case, particularly when there is substantial condensation of polychlorosilanes.

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