Ultrafast laser processing has recently emerged as a new tool for processing fiber-reinforced polymer (FRP) composites. In the astronautic industry, the modified epoxy resin (named 4211) and the modified cyanate ester resin (known as BS-4) are two of the most widely used polymers for polymer-based composites. To study the removal mechanism and ablation process of different material components during the ultrafast laser processing of FRPs, we isolated the role of the two important polymers from their composites by studying their femtosecond UV laser (260 fs, 343 nm) ablation characteristics for controllable machining and understanding the related mechanisms. Intrinsic properties for the materials’ transmission spectrum, the absorption coefficient and the optical bandgap (Eg), were measured, derived, and compared. Key parameters for controllable laser processing, including the ablation threshold (Fth), energy penetration depth (δeff), and absorbed energy density (Eabs) at the ablation threshold, as well as their respective “incubation” effect under multiple pulse excitations, were deduced analytically. The ablation thresholds for the two resins, derived from both the diameter-regression and depth-regression techniques, were compared between resins and between techniques. An optical bandgap of 3.1 eV and 2.8 eV for the 4211 and BS-4 resins, respectively, were obtained. A detectable but insignificant-to-ablation difference in intrinsic properties and ablation characteristics between the two resins was found. A systematic discrepancy, by a factor of 30~50%, between the two techniques for deriving ablation thresholds was shown and discussed. For the 4211 resin ablated by a single UV laser pulse, a Fth of 0.42 J/cm2, a δeff of 219 nm, and an Eabs of 18.4 kJ/cm3 was suggested, and they are 0.45 J/cm2, 183 nm, and 23.2 kJ/cm3, respectively, for the BS-4 resin. The study may shed light on the materials’ UV laser processing, further the theoretical modeling of ultrafast laser ablation, and provide a reference for the femtosecond UV laser processing characteristics of FRPs for the future.
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