For photopolymers, knowing the rate of diffusion of the active monomer is important when modeling the material evolution during recording in order to understand and optimize their performance. Unfortunately, a confusingly wide range of values have been reported in the literature. Re-examining these results, experiments are carried out for both coverplated (sealed) and uncoverplated material layers and the measurements are analyzed using appropriate models. In this way, a more detailed analysis of the diffraction processes taking place for large-period gratings is provided. These results, combined with those in Part II, provide unambiguous evidence that the monomer diffusion rate in a commonly used acrylamide polyvinyl alcohol-based material is of the order of 10−10 cm2=s. This value closely agrees with the predictions of the nonlocal polymerization-driven diffusion model.