AbstractThis research makes an investigation into the etching mechanism of atmospheric plasma conditions on the surface of polyethylene terephthalate (PET) films. Two types of untreated PET films (S/200 and S/500) were exposed to plasma for 0 to 5.0 min in 30‐s increments. The first set of each film type was treated in helium plasma, while the second was treated in oxygenated‐helium plasma. Differential Scanning Calorimetry (DSC) was used to characterize pre‐ and post‐exposure films. Weight changes and the degree of solubility were also determined. Based on peak area results, the percent crystallinity of PET S/200 increased by an average of 4.57% (helium treated) and 13.56% (oxygenated‐helium treated), while the S/500 showed only a small increase. There was no significant change in the melting or crystallization temperatures of either film type, indicating a decrease in amorphous content versus an increase in crystalline material. Weight loss analysis supports this theory. Solubility testing revealed a continual decrease in swelling as exposure time was increased. A model was developed to predict the change in the degree of solubility for polyphase surfaces considering the etching rate per phase. The model was applied to PET with good correlation between the model and experimental data. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 94: 2383–2389, 2004