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The accurate quantification and control of mixture stoichiometry is critical in many applications using new combustion strategies and fuels (e.g., homogeneous charge compression ignition, gasoline direct injection, and oxygenated fuels). The parameter typically used to quantify mixture stoichiometry (i.e., the proximity of a reactant mixture to its stoichiometric condition) is the equivalence ratio, ϕ. The traditional definition of ϕ is based on the relative amounts of fuel and oxidizer molecules in a mixture. This definition provides an accurate measure of mixture stoichiometry when the fuel molecule does not contain oxidizer elements and when the oxidizer molecule does not contain fuel elements. However, the traditional definition of ϕ leads to problems when the fuel molecule contains an oxidizer element, as is the case when an oxygenated fuel is used, or once reactions have started and the fuel has begun to oxidize.