Ion irradiation of polymer films is a promising process technology for photonics applications that require flexible, lightweight devices resistant to selected environmental variables. Crossed phase gratings that may serve as laser-beam array generators are fabricated using the dry process of irradiation of acrylic (PMMA) films with various doses of high-energy alpha particles through a stencil mask. The gratings are examined with the aid of AFM and SEM images, and Raman-Nath diffraction analysis is applied to estimate the generated refractive-index modulation as a function of the dose. SEM images suggest a mechanism of unsaturated bond formation and accompanying contraction of the irradiated polymer. Post-irradiation baking is shown to increase the contraction or generated surface relief by around an order of magnitude. Since the index modulation and surface relief due to irradiation tend to cancel, the overall diffraction efficiencies of unbaked gratings do not surpass 67%, although baked gratings can provide higher diffraction efficiencies.