Drying effects in 14 natural lesions were studied with quantitative light-induced fluorescence and optical pathlength spectroscopy. Results were compared with clinical judgments of the lesion surface and microradiographical characterizations of the lesions. Relative fluorescence and average pathlength decreased as a function of drying time with a decay time ranging from 35.5 to <1 min. Depth and mineral loss correlated with average pathlength total changes (r = -0.79/-0.60, respectively) and poorly with total fluorescence changes (r approximately = 0.3). The decay time of the drying process for the relative fluorescence correlated well with a theoretical model based on water diffusion in lesion and surface layer, but only for large decay times. Clinical judgments could not be related to the surface layer properties or the changes in the average pathlength, but were weakly related to the changes in the relative fluorescence. We conclude that (i) fluorescence effects are mostly due to the screening by the lesion of the fluorescence from the dentin and enamel-dentin junction; (ii) water evaporation in lesions conforms to the diffusion laws only in large lesions with low surface layer penetrability; (iii) the evaporation process is controlled by the surface layer only for small surface penetrabilities (approximately 0.1 vol% microm(-1)).