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The relationship between combustion processes and engine-out soot was investigated in an optically accessible DI diesel engine using diethylene glycol diethyl ether (DGE) fuel, a viable diesel oxygenate. The high oxygen content of DGE enables operation without soot emissions at higher loads than with a hydrocarbon fuel. The high cetane number of DGE enables operation at charge-gas temperatures below those required for current diesel fuels, which may be advantageous for reducing NOx emissions. In-cylinder optical measurements of flame lift-off length and natural luminosity were obtained simultaneously with engine-out soot measurements while varying charge-gas density and temperature. The local mixture stoichiometry at the lift-off length was characterized by a parameter called the oxygen ratio that was estimated from the measured flame lift-off length using an entrainment correlation for non-reacting sprays.