Smooth poly(methyl methacrylate) (PMMA) films without any droplets were pulsed laser deposited at a wavelength of 248 nm and a laser fluence of 125 mJ/cm 2 . After deposition at room temperature, the films possess low universal hardness of only 3 N/mm 2 . Thermal treatments up to 200°C, either during deposition or afterwards, lead to film hardening up to values of 200 N/mm 2 . Using a combination of complementary methods, two main mechanisms could be made responsible for this temperature induced hardening effect well above the glass transition temperature of 102°C. The first process is induced by the evaporation of chain fragments and low molecular mass material, which are present in the film due to the ablation process, leading to an increase of the average molecular mass and thus to hardening. The second mechanism can be seen in partial cross-linking of the polymer film as soon as chain scission occurs at higher temperatures and the mobility and reactivity of the polymer material is high enough.
Pulsed laser deposition (PLD) at 248 nm in ultra high vacuum was used to produce thin poly(methyl methacrylate) (PMMA) and poly(ethyl methacrylate) (PEMA) films. The ablation and deposition mechanisms were found to be similar in both systems. Having the same backbone, these polymers differ in the size of their polar side groups leading to changes in their dynamics. Studies of the relaxation processes were performed using mechanical torsion and bending spectroscopy by means of a doublepaddle oscillator (DPO) and an in-situ plasma plume excited reed (PPXR), respectively. A strong increase of the mechanical damping was observed during annealing of the polymer films well above the glass transition temperature T g , while in-situ X-ray measurements did not reveal any structural changes. For PEMA, the glass transition temperature T g = 335 K and the main absorption maximum appear at lower temperatures compared to PMMA (T g = 380 K), allowing one to measure the mechanical properties in a much wider range above T g .
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