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Autoignition in the homogeneous charge compression ignition (HCCI) process typically exhibits heat release in two stages called cool flame and thermal flame. The mechanisms governing these two stages were investigated using a DME-fueled HCCI engine and numerical simulations. Composition analysis after cool flame showed that the cool flame is explained by a chain reaction mechanism in which the chain terminator is the intermediate species formed in cool flame. In the case of thermal flame, although the chain reaction mechanism is complex, the behavior is clearly described by thermal explosion theory in which the rate-determining reaction is H2O2 decomposition.