Operating Organic Electronics via Aqueous Electric Double Layers

Abstract: The field of organic electronics emerged in the 1970s with the discovery of conducting polymers. With the introduction of plastics as conductors and semiconductors came many new possibilities both in production and function of electronic devices. Polymers can often be processed from solution and their softness provides both the possibility of working on flexible substrates, and various advantages in interfacing with other soft materials, e.g. biological samples and specimens. Conducting polymers readily partake in chemical and electrochemical reactions, providing an opportunity to develop new electrochemicallydriven devices, but also posing new problems for device engineers.The work of this thesis has focused on organic electronic devices in which aqueous electrolytes are an active component, but still operating in conditions where it is desirable to avoid electrochemical reactions. Interfacing with aqueous electrolytes occurs in a wide variety of settings, but we have specifically had biological environments in mind as they necessarily involve the presence of water. The use of liquid electrolytes also provides the opportunity to deliver and change the device electrolyte continuously, e.g. through microfluidic systems, which could then be used as a dynamic feature and/or be used to introduce and change analytes for sensors. Of particular interest is the electric double layer at the interface between the electrolyte and other materials in the device,  specifically its sensitivity to charge reorganization and high capacitance.The thesis first focuses on organic field effect transistors gated through aqueous electrolytes. These devices are proposed as biosensors with the transistor architecture providing a direct transduction and amplification so that it can be electrically read out. It is discussed both how to distinguish between the various operating mechanisms in electrolyte thin film transistors and how to choose a strategy to achieve the desired mechanism. Two different strategies to suppress ion penetration into, and thus electrochemical doping of, the organic semiconductor are presented.The second focus of the thesis is on polarization of ferroelectric polymer films through electrolytes. A model for the interaction between the remnant ferroelectric charge in the polymer film and the mobile ionic charges of the electrolyte is presented, and verified experimentally. The reorientation of the ferroelectric polarization via the electric double layer is also demonstrated in a regenerative medicine application; the ferroelectric polarization is shown to affect cell binding, and is used as a gentle method to nondestructively detach cells from a culture substrate.