Issue 24, 2023

Simulation of polymeric mixed ionic and electronic conductors with a combined classical and quantum mechanical model

Abstract

In organic polymeric materials with mixed ionic and electronic conduction (OMIEC), the excess charge in doped polymers is very mobile and the dynamics of the polymer chain cannot be accurately described with a model including only fixed point charges. Ions and polymer are comparatively slower and a methodology to capture the correlated motions of excess charge and ions is currently unavailable. Considering a prototypical interface encountered in this type of materials, we constructed a scheme based on the combination of MD and QM/MM to evaluate the classical dynamics of polymer, water and ions, while allowing the excess charge of the polymer chains to rearrange following the external electrostatic potential. We find that the location of the excess charge varies substantially between chains. The excess charge changes across multiple timescales as a result of fast structural fluctuations and slow rearrangement of the polymeric chains. Our results indicate that such effects are likely important to describe the phenomenology of OMIEC, but additional features should be added to the model to enable the study of processes such as electrochemical doping.

Graphical abstract: Simulation of polymeric mixed ionic and electronic conductors with a combined classical and quantum mechanical model

Supplementary files

Article information

Article type
Paper
Submitted
30 11 2022
Accepted
31 1 2023
First published
31 1 2023
This article is Open Access
Creative Commons BY license

J. Mater. Chem. C, 2023,11, 8062-8073

Simulation of polymeric mixed ionic and electronic conductors with a combined classical and quantum mechanical model

A. Landi, M. Reisjalali, J. D. Elliott, M. Matta, P. Carbone and A. Troisi, J. Mater. Chem. C, 2023, 11, 8062 DOI: 10.1039/D2TC05103F

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