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Computational Approaches for Chemistry Under Extreme Conditions pp 53–70Cite as

Accelerated Molecular Dynamics Simulations of Shock-Induced Chemistry: Application to Liquid Benzene

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Part of the book series: Challenges and Advances in Computational Chemistry and Physics ((COCH,volume 28))

Abstract

Shock-induced phenomena in materials occur on timescales that while short may still be beyond the reach of traditional molecular dynamics simulations. The shock-induced chemistry of liquid benzene provides an excellent example of the importance of timescale in shock experiments; reactions are seen at about 13.3 GPa on microsecond timescales in plate impact experiments but it appears inert at up to 20 GPa over 100s of picoseconds during laser-driven shock experiments. We have studied the shock-induced chemistry of liquid benzene using a semiempirical reactive interatomic potential at timescales beyond those routinely accessible to traditional molecular dynamics simulations. We have applied replica-based accelerated molecular dynamics to this system because the initial chemical reactions themselves can be viewed as rare, state-to-state transitions that take place under thermal activation. Replica-based accelerated molecular dynamics enables us to parallelize the simulations in time with no loss of accuracy, provided that transitions (reactions) can be detected reliably. We have simulated the shocked chemical dynamics of benzene on timescales up to 7.7 ns with high parallel efficiency. The simulations show the formation dimers through Diels–Alder condensation. The dimers subsequently condense into larger polymeric structures, in good accord with experiments and quantum chemical data.

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Acknowledgements

This work was supported by the Laboratory Directed Research and Development program of Los Alamos National Laboratory. We thank Josh Coe, Dana Dattelbaum, Shawn McGrane, Anders Niklasson, Danny Perez, Kyle Ramos, and Art Voter for many illuminating discussions over the course of this work.

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Authors and Affiliations

  1. Los Alamos National Laboratory, Los Alamos, NM, 87545, USA

    E. Martínez, E. M. Kober & M. J. Cawkwell

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  1. E. Martínez
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  2. E. M. Kober
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  3. M. J. Cawkwell
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Correspondence to M. J. Cawkwell .

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  1. Materials Science Division, Lawrence Livermore National Laboratory Materials Science Division, Livermore, CA, USA

    Nir Goldman

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Martínez, E., Kober, E.M., Cawkwell, M.J. (2019). Accelerated Molecular Dynamics Simulations of Shock-Induced Chemistry: Application to Liquid Benzene. In: Goldman, N. (eds) Computational Approaches for Chemistry Under Extreme Conditions. Challenges and Advances in Computational Chemistry and Physics, vol 28. Springer, Cham. https://doi.org/10.1007/978-3-030-05600-1_3

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