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Partially premixed combustion (PPC) is an operating mode that lies between the conventional compression ignition (CI) mode and homogeneous charge compression ignition (HCCI) mode. The combustion in this mixed mode is complex as it is neither diffusion-controlled (CI mode) nor governed solely by chemical kinetics (HCCI mode). In this study, CFD simulations were performed to evaluate flame index, which distinguishes between zones having a premixed flame and non-premixed flame. Experiments performed in the optical engine supplied data to validate the model. In order to realize PPC, the start of injection (SOI) was fixed at −40 CAD (aTDC) so that a required ignition delay is created to premix air/fuel mixture. The reference operating point was selected to be with 3 bar IMEP and 1200 rpm. Naphtha with a RON of 77 and its corresponding PRF surrogate were tested. The simulations captured the general trends observed in the experiments well.