Quantum Simulations of Radiation Damage in a Molecular Polyethylene Analog

Troup, Nathaniel; Kroonblawd, Matthew P.; Donadio, Davide; Goldman, Nir

doi:10.1002/marc.202400669

Title: Quantum Simulations of Radiation Damage in a Molecular Polyethylene Analog

Journal Article · 21 October 2024 · Macromolecular Rapid Communications

DOI: https://doi.org/10.1002/marc.202400669 · OSTI ID:2473172

Troup, Nathaniel ^[1]; Kroonblawd, Matthew P. ^[2];

^[3];

^[4]

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
Department of Chemistry University of California Davis One Shields Avenue Davis CA 95616 USA
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

Abstract 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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2473172

Journal Information:: Macromolecular Rapid Communications, Journal Name: Macromolecular Rapid Communications Journal Issue: 24 Vol. 45; ISSN 1022-1336

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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