Charge Conduction in Polymer Dielectrics: Theoretical Perspectives and First-Principle Approaches

This review highlights the updated picture of charge transport in polymer dielectrics and offers suggestions for future research. It begins with the backgrounds of the various theoretical charge transport models and the underlying concepts of the physical quantities. The techniques for deriving the microscopic physical quantities, e.g., the Marcus parameters and the spectral density of bath, from first-principles methods are outlined for tutorial purposes. Our recent multi-scale simulation studies are presented to demonstrate how and why the macroscopic charge transfer behavior can be predicted from these microscopic quantities, without the use of phenomenological/ empirical models nor ad hoc parameters. Some new insights gained through the multiscale modeling technique are summarized, with a focus on the relation between the chemical structure of polymers and the carrier transport properties. Finally, what is further required for computer-aided (rational) dielectric polymer design is discussed.