Explicit Polarization in Coarse-Grained Simulations of Ionomer Melts
Abstract
The structure and morphology of ionic aggregates in ionomer melts significantly influence their ion transport properties. Understanding the underlying mechanisms and relevant time scales of ion transport can facilitate design of viable ionomer materials as single-ion conductors for energy applications. Previous studies have characterized the ionic aggregate structure, morphology, and dynamics using non-polarizable coarse-grained molecular dynamics (CGMD) simulations. In this work, we examine the role of polarization in ionomer melts by explicitly incorporating Drude oscillators in CGMD simulations. We systematically study the structure and dynamics of pendant ionomers, focusing on the comparison to non-polarizable systems. Polarization within the ion clusters leads to less overall ion structuring. On the aggregate scale, less ion structuring yields smaller ionic aggregates. The extent to which the clusters are smaller delicately depends on the strength of the electrostatic interactions (the dielectric constant). Under certain conditions, we find that the time scale for free counterion diffusion does not depend on the morphology, unlike that in a non-polarizable model.
Additional Information
The authors thank Karen Winey and Mark Stevens for helpful discussions. C.B. is supported by the U.S. Department of Energy, Office of Science, Office of Advanced Scientific Computing Research, Department of Energy Computational Science Graduate Fellowship, under award number DE-SC0020347. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. DOE's National Nuclear Security Administration under contract DE-NA-0003525. The views expressed in the article do not necessarily represent the views of the U.S. DOE or the United States Government.Additional details
- Eprint ID
- 117908
- Resolver ID
- CaltechAUTHORS:20221117-155838300.14
- DE-SC0020347
- Department of Energy (DOE)
- DE-NA-0003525
- Department of Energy (DOE)
- Created
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2022-11-30Created from EPrint's datestamp field
- Updated
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2023-01-25Created from EPrint's last_modified field