Non-Adiabatic Quantum Molecular Dynamics Investigation of Hot Carrier Dynamics in Dielectric Polymers under High Electric Fields.

ORAL

Abstract

Non-Adiabatic Quantum Molecular Dynamics (NAQMD) is a powerful tool typically used to model excited state electron-phonon dynamics under optical excitation. In this work we have ported NAQMD to study excited hot charge carriers involved in dielectric break down of organic polymers under high electric fields. Organic polymers offer many advantages over inorganic dielectrics, but they are severely limited by break down under the application of high electric fields. There also remains no mechanistic method for quantitative prediction of the breakdown field in polymers, unlike inorganic materials. Here we performed a systematic study of different electric fields on hot carrier dynamics and resulting chemical damage in a slab of archetypal polymer, polyethylene. We found a critical transition occurring near the experimentally reported intrinsic breakdown field marked by strong localization of electronic states at the slab surface and emergence of hot carrier C-H vibrational resonance. Such a localization transition may provide a critically-missing prediction method for computationally screening dielectric polymers with high breakdown fields.

*This work was supported by the Office of Naval Research through a Multi-University Research Initiative (MURI) grant (N00014-17-1-2656).

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Presenters

  • Thomas Linker

    • Collaboratory for Advanced Computing and Simulations, University of Southern California

Authors

  • Thomas Linker

    • Collaboratory for Advanced Computing and Simulations, University of Southern California

  • Subodh Tiwari

    • Univ of Southern California
    • Collaboratory for Advanced Computing and Simulations, University of Southern California

  • Hiroyuki Kumazoe

    • Department of Physics, Kumamoto University

  • Shogo Fukushima

    • Kumamoto University
    • Department of Physics, Kumamoto University

  • Rajiv Kalia

    • Mork Family Department of Chemical Engineering and Materials Science, University of Southern California
    • Univ of Southern California
    • Collaboratory for Advanced Computing and Simulations, University of Southern California

  • Aiichiro Nakano

    • Mork Family Department of Chemical Engineering and Materials Science, University of Southern California
    • Univ of Southern California
    • Collaboratory for Advanced Computing and Simulations, University of Southern California

  • Ramamurthy Ramprasad

    • Georgia Institute of Technology
    • School of Materials Science and Engineering, Georgia Institute of Technology
    • Department of Material Science and Technology, Georgia Tech
    • Materials Science and Engineering, Georgia Institute of Technology

  • Fuyuki Shimojo

    • Department of Physics, Kumamoto University
    • Kumamoto University

  • Priya Vashishta

    • Mork Family Department of Chemical Engineering and Materials Science, University of Southern California
    • Univ of Southern California
    • University of Southern California
    • Collaboratory for Advanced Computing and Simulations, University of Southern California