Three types of human odontogenic tumors histologically classified as compound composite odontoma, ossifying fibroma, and Pindborg tumor were characterized using mid-infrared spectroscopy (mid-IR) and solid-state nuclear magnetic resonance (ssNMR). For comparison, human jawbone and dental mineralized tissues such as dentin, enamel, and dental cement were also characterized. The studies focused on the structural properties and chemical composition of pathological tissues versus histochemically related tissues. All analyzed tumors were composed of organic and mineral parts and water. Apatite was found to be the main constituent of the mineral part. Various components (water, structural hydroxyl groups, carbonate ions (CO<sub>3</sub><sup>2−</sup>), and hydrogen phosphate ions (HPO<sub>4</sub><sup>2−</sup>)) and physicochemical parameters (index of apatite maturity and crystallinity) were examined. The highest organic/mineral ratio was observed in fibrocementoma, a finding that can be explained by the fibrous character of the tumor. The lowest relative HPO<sub>4</sub><sup>2−</sup> content was found in odontoma. This tumor is characterized by the highest mineral crystallinity index and content of structural hydroxyl groups. The Pindborg tumor mineral portion was found to be poorly crystalline and rich in HPO<sub>4</sub><sup>2−</sup>. The relative CO<sub>3</sub><sup>2−</sup> content was similar in all samples studied. The results of spectroscopic studies of odontogenic tumors were consistent with the standard histochemical analysis. It was shown that the various techniques of ssNMR and elaborate analysis of the mid-IR spectra, applied together, provide valuable information about calcified benign odontogenic tumors.

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