Publication date: 11th March 2026
Semiconducting polymers interfaced with electrolytes are finding wide interest across a range of energy generation and storage and sensing technologies, including as photoelectrodes for chemical energy production, electrodes for energy storage, and the active matrix in biochemical sensors. How the physicochemical nature of the interphase between soft semiconducting polymers and electrolytes change as a function of the chemistries of these components, swelling, applied electric fields, and charge-carrier injection into the polymer remain outstanding questions that need to be resolved to design materials that can achieve efficient charge and ion transport. Here we will discuss recent advances in understanding the formation and dynamics of the polymer–electrolyte interphase through the development of multiscale modeling approaches. Quantum chemical calculations are used to describe the nature of the charge carriers (i.e., polarons and bipolarons) in the semiconducting polymers, including how the dielectric environment and interactions with counterions impact charge-carrier (de)localization and the resulting optical response. We then develop and deploy molecular dynamics (MD) simulations to examine dynamic features of polymer swelling by the electrolyte as a function of applied electric fields and charge-carrier injection into the polymer.
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