This study aims to improve the understanding of the effect of both calcination temperature and the carbonation process on cement pastes by analyzing the Fourier-transform infrared spectroscopy (FTIR) principal vibration modes. In this regard, six samples of cement pastes, identified as (CS1, CS2, CS3, CS4, CS5 and CS6), mixed with white sugar with different concentrations (X = 0, 0.2, 0.4, 0.6, 0.8, and 1.1 %), respectively, were prepared. These blended cement samples were heated (calcined) at a temperature of about 600°C. Moreover, an additional sugar-free sample tagged as CS0 was prepared and cured at room temperature for 7 days. Afterward, these samples were subjected to FTIR spectroscopy and X-ray diffraction to investigate the effect of the calcination and the carbonation process on the principal mode of vibrations and the microstructure of the ordinary Portland cement (OPC) matrix as well. The characteristics of the FTIR principal modes of vibrations were investigated. Besides, the relaxation time and the rotational energy barrier were calculated for different sugar concentrations. This study revealed that the kinetic reaction of the carbon contained in the different samples with the C 3 S, C 2 S, C-S-H and CH phases leads to the formation of calcium carbonate CaCO 3 , where the rate of formation depends upon the carbonation rate of samples. The critical variation for the relaxation time and rotational energy barrier clearly appeared at X = 0.6%. Moreover, the kinetic carbonation of both clinker phases and the hydrated phases in the OPC matrix system mainly depends upon the rate of the polymerization of the silicate group inside the matrix of OPC.