Quantum Simulations of Radiation Damage in a Molecular Polyethylene Analog.

Autor: Troup N; Department of Chemical Engineering, University of California Davis, One Shields Avenue, Davis, CA, 95616, USA., Kroonblawd MP; Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, 94550, USA., Donadio D; Department of Chemistry, University of California Davis, One Shields Avenue, Davis, CA, 95616, USA., Goldman N; Department of Chemical Engineering, University of California Davis, One Shields Avenue, Davis, CA, 95616, USA.; Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, 94550, USA.
Jazyk: angličtina
Zdroj: Macromolecular rapid communications [Macromol Rapid Commun] 2024 Dec; Vol. 45 (24), pp. e2400669. Date of Electronic Publication: 2024 Oct 22.
DOI: 10.1002/marc.202400669
Abstrakt: An atomic-level understanding of radiation-induced damage in simple polymers like polyethylene is essential for determining how these chemical changes can alter the physical and mechanical properties of important technological materials such as plastics. Ensembles of quantum simulations of radiation damage in a polyethylene analog are performed using the Density Functional Tight Binding method to help bind its radiolysis and subsequent degradation as a function of radiation dose. Chemical degradation products are categorized with a graph theory approach, and occurrence rates of unsaturated carbon bond formation, crosslinking, cycle formation, chain scission reactions, and out-gassing products are computed. Statistical correlations between product pairs show significant correlations between chain scission reactions, unsaturated carbon bond formation, and out-gassing products, though these correlations decrease with increasing atom recoil energy. The results present relatively simple chemical descriptors as possible indications of network rearrangements in the middle range of excitation energies. Ultimately, the work provides a computational framework for determining the coupling between nonequilibrium chemistry in polymers and potential changes to macro-scale properties that can aid in the interpretation of future radiation damage experiments on plastic materials.
(© 2024 The Author(s). Macromolecular Rapid Communications published by Wiley‐VCH GmbH.)
Databáze: MEDLINE
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