Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.035
Publication date: 18th July 2023
The charge-transport properties of conjugated polymers have been studied intensively for both electronic and optoelectronic device applications. Some polymer semiconductors not only support the ambipolar transport of electrons and holes, but do so with comparable carrier mobilities. This opens the possibility of gaining deeper insight into the charge-transport physics of these complex materials via comparison between electron and hole dynamics while keeping other factors, such as polymer microstructure or vibrational fluctuations, equal. Field-induced electron spin resonance spectroscopy has been recently used to compare the spin relaxation behavior of electron and hole polarons in three ambipolar conjugated polymers, showing three spin relaxation regimes as a function of temperature. We interpret these findings on the basis of calculated electronic structure calculations and state-of-the-art numerical propagation of the hole and electron carrier wavefunctions coupled to nuclear motion in these polymers.
In the second part of the talk, we will report on recent simulations of ion intake and diffusion in crystalline microstructures of conjugated polymers equipped with glycolated side chains for organic electrochemical transistor applications. All-atom simulations support a crystal phase transition upon doping that occurs via a zipping mechanism. We will also describe preliminary phenomenological calculations aiming at describing the changes in electrical conductivity with increasing carrier concentration and that take into account the electrostatic interactions with the ions.