Atomistic mechanisms for chemical defects formation in polyethylene

Chemical defects can progressively degrade the electronic structure of polymer dielectrics, ultimately leading to their failure. Because the polymer degradation and breakdown related processes are notably complicated in nature, they remain far from being understood both experimentally and computationally. Using a combination of density functional theory calculations and classical molecular dynamics simulations, we propose seven atomistic mechanisms for the formation of common chemical defects in polyethylene using which a variety of defect-related experimental observations can be explained. This work provides a comprehensive connection among the experiments related to polyethylene defects and aging, laying the groundwork for an understanding of polymer degradation and breakdown.