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The oxynitride materials present a high versatility, which enables their properties to be controlled by tuning their elemental composition. This is the case for silicon oxynitrides used for multilayer antireflective coatings (ARCs), where several thin films with various refractive indexes are needed. Different techniques allow for the modification of the thin film composition. In this paper, we investigate the reactive gas pulsing sputtering process to easily tune the thin film composition, from an oxide to a nitride, by controlling the averaged oxygen flow rate, without reducing the deposition rate, compared to a conventional reactive process (CP). We then demonstrated that the refractive indexes of films deposited by this pulsing process (PP) can be varied in the same range compared to films obtained by CP (from 1.83 to 1.45 at 1.95 eV), whereas their extinction coefficients remain low. Finally, the multilayer ARC has been simulated and optimized by a genetic algorithm for wavelength at 600 nm and for the silicon substrate. Various optimized multilayer (mono-, bi- and tri-layers) structures have been deposited by the PP technique and characterized. They are presented in good agreement with the simulated reflectivity. Hence, the PP allows for an easy depositing tri-layer system with a reasonable deposition rate and low reflectivity (8.1% averaged on 400–750 nm visible light range). [ABSTRACT FROM AUTHOR]