Multiscale Strategy for Predicting Radiation Chemistry in Polymers

Kroonblawd, Matthew P.; Yoshimura, Anthony; Goldman, Nir; Maiti, Amitesh; Lewicki, James P.; Saab, Andrew P.

doi:10.1021/acs.jctc.2c00582

Title: Multiscale Strategy for Predicting Radiation Chemistry in Polymers

Journal Article · 12 August 2022 · Journal of Chemical Theory and Computation

DOI: https://doi.org/10.1021/acs.jctc.2c00582 · OSTI ID:1994025

^[1];

^[2];

^[1];

^[1]; Saab, Andrew P. ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); University of California, Davis, CA (United States)

A primary mode for radiation damage in polymers arises from ballistic electrons that induce electronic excitations, yet subsequent chemical mechanisms are poorly understood. We develop a multiscale strategy to predict this chemistry starting from subatomic scattering calculations. Nonadiabatic molecular dynamics simulations sample initial bond-breaking events following the most likely excitations, which feed into semiempirical simulations that approach chemical equilibrium. Application to polyethylene reveals a mechanism explaining the low propensity to cross-link in crystalline samples.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1994025

Report Number(s):: LLNL-JRNL-834986; 1053702

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 9 Vol. 18; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (63)

Zur Theorie des Durchgangs schneller Elektronen durch Materie Møller, Chr. Annalen der Physik, Vol. 406, Issue 5 https://doi.org/10.1002/andp.19324060506	journal	January 1932
Temperature Dependence of Structural Properties and Chain Configurational Study: A Molecular Dynamics Simulation of Polyethylene Chains Lu, Haifeng; Zhou, Zhiping; Hao, Tongfan Macromolecular Theory and Simulations, Vol. 24, Issue 4 https://doi.org/10.1002/mats.201500007	journal	April 2015
Effect of physical state during the electron irradiation of hydrocarbon polymers. Part I. The influence of physical state on reactions occurring in polyethylene during and following the irradiation Lawton, Elliott J.; Balwit, J. S.; Powell, R. S. Journal of Polymer Science, Vol. 32, Issue 125 https://doi.org/10.1002/pol.1958.1203212501	journal	November 1958
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
The Interaction of Radiation with Matter Bichsel, Hans; Schindler, Heinrich Particle Physics Reference Library https://doi.org/10.1007/978-3-030-35318-6_2	book	January 2020
Relativistic collisions: The work of Christian M�ller in the early 1930s Kragh, Helge Archive for History of Exact Sciences, Vol. 43, Issue 4 https://doi.org/10.1007/BF00374762	journal	January 1992
M�ller scattering: a neglected application of early quantum electrodynamics Roqu�, Xavier Archive for History of Exact Sciences, Vol. 44, Issue 3 https://doi.org/10.1007/BF00377049	journal	January 1992
The influence of polarization functions on molecular orbital hydrogenation energies Hariharan, P. C.; Pople, J. A. Theoretica Chimica Acta, Vol. 28, Issue 3 https://doi.org/10.1007/BF00533485	journal	January 1973
Radiation damage and electron microscopy of organic polymers Grubb, D. T. Journal of Materials Science, Vol. 9, Issue 10 https://doi.org/10.1007/BF00540772	journal	October 1974
Radiation effects in polyethylene and n-alkanes Ungar, G. Journal of Materials Science, Vol. 16, Issue 10 https://doi.org/10.1007/BF02402826	journal	October 1981
Polymeric composite materials for radiation shielding: a review More, Chaitali V.; Alsayed, Zainab; Badawi, Mohamed. S. Environmental Chemistry Letters, Vol. 19, Issue 3 https://doi.org/10.1007/s10311-021-01189-9	journal	February 2021
Gamma Irradiation of Silicones Palsule, Aniruddha S.; Clarson, Stephen J.; Widenhouse, Christopher W. Journal of Inorganic and Organometallic Polymers and Materials, Vol. 18, Issue 2 https://doi.org/10.1007/s10904-008-9205-0	journal	April 2008
Crystal structure analysis of polyethylene with electron diffraction intensity data: Deconvolution of multiple scattering effects Dorset, Douglas L.; Moss, Barbara Polymer, Vol. 24, Issue 3 https://doi.org/10.1016/0032-3861(83)90265-3	journal	March 1983
Ion bombardment of polyethylene Beardmore, Keith; Smith, Roger Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 102, Issue 1-4 https://doi.org/10.1016/0168-583X(95)80145-C	journal	August 1995
3D inkjet-printed UV-curable inks for multi-functional electromagnetic applications Saleh, Ehab; Woolliams, Peter; Clarke, Bob Additive Manufacturing, Vol. 13 https://doi.org/10.1016/j.addma.2016.10.002	journal	January 2017
Optimization algorithm for the generation of ONCV pseudopotentials Schlipf, Martin; Gygi, François Computer Physics Communications, Vol. 196 https://doi.org/10.1016/j.cpc.2015.05.011	journal	November 2015
Extensive TD-DFT investigation of the first electronic transition in substituted azobenzenes Jacquemin, Denis; Perpète, Eric A.; Scuseria, Gustavo E. Chemical Physics Letters, Vol. 465, Issue 4-6 https://doi.org/10.1016/j.cplett.2008.09.071	journal	November 2008
Coupling effects of gamma irradiation and absorbed moisture on silicone foam Wang, Pu-Cheng; Yang, Na; Liu, Dong Materials & Design, Vol. 195 https://doi.org/10.1016/j.matdes.2020.108998	journal	October 2020
Irradiation effects in high-density polyethylene Polvi, Jussi; Nordlund, Kai Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 312 https://doi.org/10.1016/j.nimb.2013.07.002	journal	October 2013
Comparison of low-energy β radiation effects in polyethylene and cellulose by molecular dynamics simulations Polvi, Jussi; Nordlund, Kai Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 326 https://doi.org/10.1016/j.nimb.2013.10.047	journal	May 2014
Overview of accelerated aging and polymer degradation kinetics for combined radiation-thermal environments Celina, Mathew; Linde, Erik; Brunson, Douglas Polymer Degradation and Stability, Vol. 166 https://doi.org/10.1016/j.polymdegradstab.2019.06.007	journal	August 2019
All-atomic and coarse-grained molecular dynamics investigation of deformation in semi-crystalline lamellar polyethylene Olsson, Pär A. T.; in ’t Veld, Pieter J.; Andreasson, Eskil Polymer, Vol. 153 https://doi.org/10.1016/j.polymer.2018.07.075	journal	September 2018
First Principles Nonadiabatic Excited-State Molecular Dynamics in NWChem Song, Huajing; Fischer, Sean A.; Zhang, Yu Journal of Chemical Theory and Computation, Vol. 16, Issue 10 https://doi.org/10.1021/acs.jctc.0c00295	journal	August 2020
A Quantum-Based Approach to Predict Primary Radiation Damage in Polymeric Networks Kroonblawd, Matthew P.; Goldman, Nir; Maiti, Amitesh Journal of Chemical Theory and Computation, Vol. 17, Issue 1 https://doi.org/10.1021/acs.jctc.0c00967	journal	December 2020
Constitutive Model of Radiation Aging Effects in Filled Silicone Elastomers under Strain Maiti, A.; Small, W.; Kroonblawd, M. P. The Journal of Physical Chemistry B, Vol. 125, Issue 35 https://doi.org/10.1021/acs.jpcb.1c04958	journal	August 2021
Chemical Degradation Pathways in Siloxane Polymers Following Phenyl Excitations Kroonblawd, Matthew P.; Goldman, Nir; Lewicki, James P. The Journal of Physical Chemistry B, Vol. 122, Issue 50 https://doi.org/10.1021/acs.jpcb.8b09636	journal	November 2018
High-Accuracy Semiempirical Quantum Models Based on a Minimal Training Set Pham, Cong Huy; Lindsey, Rebecca K.; Fried, Laurence E. The Journal of Physical Chemistry Letters, Vol. 13, Issue 13 https://doi.org/10.1021/acs.jpclett.2c00453	journal	March 2022
Gamma Radiation Chemistry of Polydimethylsiloxane Foam in Radiation-Thermal Environments: Experiments and Simulations Liu, Qiang; Huang, Wei; Liu, Bo ACS Applied Materials & Interfaces, Vol. 13, Issue 34 https://doi.org/10.1021/acsami.1c10765	journal	August 2021
UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations Rappe, A. K.; Casewit, C. J.; Colwell, K. S. Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035 https://doi.org/10.1021/ja00051a040	journal	December 1992
The OPLS [optimized potentials for liquid simulations] potential functions for proteins, energy minimizations for crystals of cyclic peptides and crambin Jorgensen, William L.; Tirado-Rives, Julian Journal of the American Chemical Society, Vol. 110, Issue 6 https://doi.org/10.1021/ja00214a001	journal	March 1988
Primary Radiation Defect Production in Polyethylene and Cellulose Polvi, Jussi; Luukkonen, Petri; Nordlund, Kai The Journal of Physical Chemistry B, Vol. 116, Issue 47 https://doi.org/10.1021/jp309979p	journal	November 2012
Polymer degradation through chemical change: a quantum-based test of inferred reactions in irradiated polydimethylsiloxane Kroonblawd, Matthew P.; Goldman, Nir; Maiti, Amitesh Physical Chemistry Chemical Physics, Vol. 24, Issue 14 https://doi.org/10.1039/D1CP05647F	journal	January 2022
Quantum theory of electronic excitation and sputtering by transmission electron microscopy Yoshimura, Anthony; Lamparski, Michael; Giedt, Joel Nanoscale, Vol. 15, Issue 3 https://doi.org/10.1039/D2NR01018F	journal	January 2023
Excitation Energy Transfer in Alkanes. I. Exciton Model Partridge, Roger H. The Journal of Chemical Physics, Vol. 52, Issue 5 https://doi.org/10.1063/1.1673332	journal	March 1970
Excitation Energy Transfer in Alkanes. II. Experimental Demonstration Partridge, Roger H. The Journal of Chemical Physics, Vol. 52, Issue 5 https://doi.org/10.1063/1.1673333	journal	March 1970
Excitation Energy Transfer in Alkanes. III. Radiation Chemistry of Alkane Polymers Partridge, Roger H. The Journal of Chemical Physics, Vol. 52, Issue 5 https://doi.org/10.1063/1.1673334	journal	March 1970
Self‐Consistent Molecular‐Orbital Methods. IX. An Extended Gaussian‐Type Basis for Molecular‐Orbital Studies of Organic Molecules Ditchfield, R.; Hehre, W. J.; Pople, J. A. The Journal of Chemical Physics, Vol. 54, Issue 2 https://doi.org/10.1063/1.1674902	journal	January 1971
Self—Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian—Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules Hehre, W. J.; Ditchfield, R.; Pople, J. A. The Journal of Chemical Physics, Vol. 56, Issue 5, p. 2257-2261 https://doi.org/10.1063/1.1677527	journal	March 1972
Experimental and Theoretical Study of Sigma‐Bond Electronic Transitions in Alkanes Raymonda, John W.; Simpson, William T. The Journal of Chemical Physics, Vol. 47, Issue 2 https://doi.org/10.1063/1.1711913	journal	July 1967
Canonical sampling through velocity rescaling Bussi, Giovanni; Donadio, Davide; Parrinello, Michele The Journal of Chemical Physics, Vol. 126, Issue 1 https://doi.org/10.1063/1.2408420	journal	January 2007
Lagrangian formulation with dissipation of Born-Oppenheimer molecular dynamics using the density-functional tight-binding method Zheng, Guishan; Niklasson, Anders M. N.; Karplus, Martin The Journal of Chemical Physics, Vol. 135, Issue 4 https://doi.org/10.1063/1.3605303	journal	July 2011
A unified formulation of the constant temperature molecular dynamics methods Nosé, Shuichi The Journal of Chemical Physics, Vol. 81, Issue 1 https://doi.org/10.1063/1.447334	journal	July 1984
Molecular dynamics with electronic transitions Tully, John C. The Journal of Chemical Physics, Vol. 93, Issue 2 https://doi.org/10.1063/1.459170	journal	July 1990
Toward reliable density functional methods without adjustable parameters: The PBE0 model Adamo, Carlo; Barone, Vincenzo The Journal of Chemical Physics, Vol. 110, Issue 13 https://doi.org/10.1063/1.478522	journal	April 1999
Nonadiabatic excited-state molecular dynamics: Treatment of electronic decoherence Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E. The Journal of Chemical Physics, Vol. 138, Issue 22 https://doi.org/10.1063/1.4809568	journal	June 2013
Molecular dynamics of polymer crystallization revisited: Crystallization from the melt and the glass in longer polyethylene Yamamoto, Takashi The Journal of Chemical Physics, Vol. 139, Issue 5 https://doi.org/10.1063/1.4816707	journal	August 2013
DFTB+, a software package for efficient approximate density functional theory based atomistic simulations Hourahine, B.; Aradi, B.; Blum, V. The Journal of Chemical Physics, Vol. 152, Issue 12 https://doi.org/10.1063/1.5143190	journal	March 2020
NWChem: Past, present, and future Aprà, E.; Bylaska, E. J.; de Jong, W. A. The Journal of Chemical Physics, Vol. 152, Issue 18 https://doi.org/10.1063/5.0004997	journal	May 2020
LXXIX. The scattering of α and β particles by matter and the structure of the atom Rutherford, E. The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 21, Issue 125 https://doi.org/10.1080/14786440508637080	journal	May 1911
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1 https://doi.org/10.1088/0965-0393/18/1/015012	journal	December 2009
The Impact of Sterilization Method on Wear in Knee Arthroplasty Williams, Ian R.; Mayor, Michael B.; Collier, John P. Clinical Orthopaedics and Related Research, Vol. 356 https://doi.org/10.1097/00003086-199811000-00024	journal	January 1998
Thermal Properties of the Inhomogeneous Electron Gas Mermin, N. David Physical Review, Vol. 137, Issue 5A https://doi.org/10.1103/PhysRev.137.A1441	journal	March 1965
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/PhysRev.140.A1133	journal	November 1965
Canonical dynamics: Equilibrium phase-space distributions Hoover, William G. Physical Review A, Vol. 31, Issue 3 https://doi.org/10.1103/PhysRevA.31.1695	journal	March 1985
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Self-consistent-charge density-functional tight-binding method for simulations of complex materials properties Elstner, M.; Porezag, D.; Jungnickel, G. Physical Review B, Vol. 58, Issue 11, p. 7260-7268 https://doi.org/10.1103/PhysRevB.58.7260	journal	September 1998
Optimized norm-conserving Vanderbilt pseudopotentials Hamann, D. R. Physical Review B, Vol. 88, Issue 8 https://doi.org/10.1103/PhysRevB.88.085117	journal	August 2013
Controlled manipulation of elastomers with radiation: Insights from multiquantum nuclear-magnetic-resonance data and mechanical measurements Maiti, A.; Weisgraber, T.; Dinh, L. N. Physical Review E, Vol. 83, Issue 3 https://doi.org/10.1103/PhysRevE.83.031802	journal	March 2011
Radiation-induced mechanical property changes in filled rubber Maiti, A.; Weisgraber, T. H.; Gee, R. H. Physical Review E, Vol. 83, Issue 6 https://doi.org/10.1103/PhysRevE.83.062801	journal	June 2011
Density-Functional Theory for Time-Dependent Systems Runge, Erich; Gross, E. K. U. Physical Review Letters, Vol. 52, Issue 12 https://doi.org/10.1103/PhysRevLett.52.997	journal	March 1984
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Chapter III. Standard Measurements of the Cobalt 60 Gamma Radiation Thoraeus, R. Acta Radiologica, Vol. 51, Issue sup179 https://doi.org/10.3109/00016925909173793	journal	January 1959

Similar Records

Multiscale simulation of polymer nanocomposites

Journal Article · 2011 · Physics of Atomic Nuclei · OSTI ID:22043820

Efficient Multiscale Optoelectronic Prediction for Conjugated Polymers

Journal Article · 2019 · Macromolecules · OSTI ID:1601973

Jackson, Nicholas E.; Bowen, Alec S.; de Pablo, Juan J.

Predictive multiscale modeling for Unidirectional Carbon Fiber Reinforced Polymers

Journal Article · 2020 · Composites Science and Technology · OSTI ID:1799256

Gao, Jiaying; Shakoor, Modesar; Domel, Gino; +5 more

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
73 NUCLEAR PHYSICS AND RADIATION PHYSICS
conformation
excited states
mathematical methods
nucleic acid structure
scattering

Title: Multiscale Strategy for Predicting Radiation Chemistry in Polymers

Citation Formats

References (63)

Similar Records

Related Subjects