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Abstract: The use of fluoride for the prevention of caries is based on the transformation of hydroxylapatite to fluoroapatite in the presence of fluoride ions, thereby strengthening tooth structure. Adhesion of dentin and resin composite (tooth-colored restoration material) requires a dentin bonding system, since resin composite is not able to adhere to dentin directly. Demineralization of dentin by acid etching is an important step in the dentin bonding system, however, demineralization also introduces weaknesses in tooth structure. If the demineralized dentin could be strengthened by the application of fluoride, then the dentin–resin composite bond strength might also improve. To test this hypothesis, the present study evaluated the influence of fluoride applications on the strength of the dentin–resin composite bond by (1) tensile strength testing analyses, (2) SEM analyses of tooth structure, and (3) detection of calcium (Ca) and fluorine (F) distribution patterns by micro proton-induced X-ray emission (μ-PIXE) and micro proton-induced gamma-ray emission (μ-PIGE) analyses conducted at the Takasaki Ion Accelerators for Advanced Radiation Application (TIARA) at the Takasaki Advanced Radiation Research Institute (TARRI). In this study, the dentin in extracted human molars was exposed by grinding and the dentin was etched with 35% phosphoric acid. Fluoride was applied at two concentrations, 0.022% (100ppm F) and 2.21% (10,000ppm F) NaF solution, for two time periods, 30 and 60s, prior to bonding the resin composite with the treated dentin. Controls were prepared in the same manner, but without the fluoride application. Bond strength was measured with a micro-tensile testing unit, and the fluorine and calcium distributions at the interface between dentin and resin composite were detected by μ-PIGE and μ-PIXE analysis, respectively. Results indicate that the 10,000ppm F applications resulted in higher bond strengths than observed in either the 100ppm F applications or the control group. In addition, PIGE analyses showed high concentrations of fluorine in the hybrid bonding layer of the 10,000ppm F samples, suggesting that the fluorine contributes to the strength of the dentin–resin composite bond. Detection of fluoroapatite within the hybrid bonding layer suggests that bond strength involves remineralization processes. [Copyright &y& Elsevier]