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The dielectric function of Ag nanoparticle films, deduced from an analysis of in situ real-time spectroscopic ellipsometry (RTSE) measurements, is found to evolve with time during deposition in close consistency with the film structure, deduced in the same RTSE analysis. In the nucleation regime, the intraband dielectric function component is absent and plasmon polariton behavior dominates. Only at nuclei contact, does the intraband amplitude appear, increasing above zero. Both intraband and plasmon amplitudes coexist during surface smoothening associated with coalescence. The intraband relaxation time increases rapidly after surface smoothening is complete, also in consistency with the thin film structural evolution.