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Abstract:We report the utility of a rapid polarization-resolved hyperspectral stimulated Raman scattering (SRS) imaging technique developed for optical diagnosis and characterization of dental caries in the tooth. Hyperspectral SRS images (512 × 512 pixels) of the tooth covering both the fingerprint (800-1800 cm −1 ) and high-wavenumber (2800-3600 cm −1 ) regions can be acquired within 15 minutes, which is at least 10 3 faster in imaging speed than confocal Raman mapping. Hyperspectral SRS imaging uncovers the biochemical distributions and variations across the carious enamel in the tooth. SRS imaging shows that compared to the sound enamel, the mineral content in the body of lesion decreases by 55%; while increasing up to 110% in the surface zone, indicating the formation of a hyper-mineralized layer due to the remineralization process. Further polarized SRS imaging shows that the depolarization ratios of hydroxyapatite crystals (ν 1 -PO 4 3-of SRS at 959 cm −1 ) of the tooth in the sound enamel, translucent zone, body of lesion and the surface zone are 0.035 ± 0.01, 0.052 ± 0.02, 0.314 ± 0.1, 0.038 ± 0.02, respectively, providing a new diagnostic criterion for discriminating carious lesions from sound enamel in the teeth. This work demonstrates for the first time that the polarization-resolved hyperspectral SRS imaging technique can be used for quantitatively determining tooth mineralization levels and discriminating carious lesions from sound enamel in a rapid fashion, proving its promising potential of early detection and diagnosis of dental caries without labeling.