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Natural gas, biogas, and biomethane are attractive fuels for compressed natural gas (CNG) engines because of their beneficial physical and chemical characteristics. This paper examines three combustion modes - homogeneous stoichiometric, homogeneous lean burn, and stratified combustion - in an optical single cylinder engine with a gas direct injection system operating with an injection pressure of 18 bar. The combustion process in each mode was characterized by indicated parameters, recording combustion images, and analysing combustion chemiluminescence emission spectra. Pure methane, which is the main component of CNG (up to 98%) or biomethane (> 98 %), was used as the fuel. Chemiluminescence emission spectrum analysis showed that OH* and CN* peaks appeared at their characteristic wavelengths in all three combustion modes. The peak of OH* and broadband CO2* intensities were strongly dependent on the air/fuel ratio conditions in the cylinder.