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Polymer thin films were deposited by laser ablation using infrared radiation both resonant (2.90, 3.40, 3.45, and 8.96 μm) and nonresonant (3.30, 3.92, and 4.17 μm) with vibrational modes in the starting material, polyethylene glycol. The chemical structure of the films was characterized by Fourier transform infrared spectroscopy, while the molecular weight distribution was investigated using gel permeation chromatography. The films deposited by resonant irradiation are superior to those deposited with nonresonant radiation with respect to both the chemical structure and the molecular weight distribution of the films. However, the molecular-weight distributions of films deposited at nonresonant infrared wavelengths show marked polymer fragmentation. Fluence and wavelength dependence studies show that the effects may be related to the degree of thermal confinement, and hence to the relative absorption strengths of the targeted vibrational modes. © 2002 American Institute of Physics.