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In this study, a spectroscopic method was used to measure the combustion characteristics of a test diesel engine when operated on dimethyl ether (DME) under a homogenous charge compression ignition (HCCI) combustion process. A numerical analysis was made of the elementary reactions using Chemkin 4.0 to perform the calculations. The results of the analysis showed that compression ratio changes and the methane additive influenced the autoignition timing in the DME-HCCI combustion process. In the experiments, reducing the compression ratio delayed the time of the peak cylinder pressure until after top dead center, thereby increasing the crankshaft output and thermal efficiency. The addition of methane enabled the DME-HCCI engine to provide crankshaft output equivalent to that seen for diesel engine operation at a low equivalence ratio. This paper discusses these effects in reference to the experimental and calculated results.