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Thin films of polyethylene glycol (MW 1500) have been prepared by pulsed-laser deposition (PLD) using both a tunable infrared (λ=2.9 μm, 3.4 μm) and an ultraviolet laser (λ=193 nm). A comparison of the physicochemical properties of the films by means of Fourier transform infrared spectroscopy, electrospray ionization mass spectrometry, and matrix-assisted laser desorption and ionization shows that when the IR laser is tuned to a resonant absorption in the polymer, the IR PLD thin films are identical to the starting material, whereas the UV PLD show significant structural modification. These results are important for several biomedical applications of organic and polymeric thin films. © 2001 American Vacuum Society.