Chemical potential–electric double layer coupling in conjugated polymer–polyelectrolyte blends

Conjugated polymer–polyelectrolyte blends combine and couple electronic semiconductor functionality with selective ionic transport, making them attractive as the active material in organic biosensors and bioelectronics, electrochromic displays, neuromorphic computing, and energy conversion and storage. Although extensively studied and explored, fundamental knowledge and accurate quantitative models of the coupled ion-electron functionality and transport are still lacking to predict the characteristics of electrodes and devices based on these blends. We report on a two-phase model, which couples the chemical potential of the holes, in the conjugated polymer, with the electric double layer residing at the conjugated polymer–polyelectrolyte interface. The model reproduces a wide range of experimental charging and transport data and provides a coherent theoretical framework for the system as well as local electrostatic potentials, energy levels, and charge carrier concentrations. This knowledge is crucial for future developments and optimizations of bioelectronic and energy devices based on the electronic-ionic interaction within these materials.