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Organic electrochemical transistors (OECTs) are highly versatile in terms of their form factor, fabrication approach that can be applied, and freedom in the choice of substrate material. Their ability to transduce ionic into electric signals and the use of bio-compatible organic materials makes them ideally suited for a wide range of applications, in particular in areas where electronic circuits are interfaced with biologic matter. OECT technology has attracted widespread interest in recent years, which has been accompanied by a steady increase in its performance. However, this progress was mainly driven by device optimization and less by targeting the design of new device geometries and OECT materials. To narrow this gap, this review provides an overview on the different device models that are used to explain the underlying physics governing the steady and transient behavior of OECTs. We show how the models can be used to identify synthetic targets to produce higher performing OECT materials and summarize recently reported materials classes. Overall, a road-map of future research in new device models and material design is presented summarizing the most pressing open questions in the understanding of OECTs. 

Doping organic semiconductors has become a key technology to increase the performance of organic light-emitting diodes, solar cells, or field-effect transistors (OFETs). However, doping can be used not only to optimize these devices but also to enable new design principles as well. Here, a novel type of OFET is reported—the vertical organic tunnel field-effect transistor. Based on heterogeneously doped drain and source contacts, charge carriers are injected from an n-doped source electrode into the channel by Zener tunneling and are transported toward a p-doped drain electrode. The working mechanism of these transistors is discussed with the help of a tunnel model that takes energetic broadening of transport states in organic semiconductors and roughness of organic layers into account. The proposed device principle opens new ways to optimize OFETs. It is shown that the Zener junction included between the source and drain of the vertical organic tunnel field-effect transistors suppresses short channel effects and improves the saturation of vertical OFETs. 

Organic electrochemical transistors (OECTs) are becoming a key device in the field of organic bioelectronics. For many applications of OECTs, in particular for enzymatic sensing, a complex mixture of room temperature ionic liquids (RTILs) combined with other electrolytes is used as a gate electrolyte, making the interpretation of experimental trends challenging. Here, the switching mechanism of OECTs using such RTILs is studied. It shows that ions smaller in size than the ions contained in the RTIL (e.g., Na+) have to be added to the ionic liquid to ensure switching of the OECTs. Furthermore, it is shown that OECTs based on RTILs exhibit noticeable gate‐bias stress effects and a hysteresis in the electrical transfer characteristics. A model based on incomplete charging/discharging of the effective gate capacitance during operation of the OECT and a dispersion in the ion mobilities is proposed to explain these instabilities, and thus it shows that the hysteresis can be minimized by optimizing the geometry of the device. Overall, a better understanding of the underlying mechanisms of switching and stability of OECTs based on RTILs is the first step toward various applications such as lactate acid sensors and neurotransmitter recording. 

Research in Organic Permeable Base Transistors (OPBTs) has led to a significant increase in their performance. However, despite this progress, understanding of the working mechanism of OPBTs is still limited. Although first numerical models of OPBTs are able to describe the switching mechanism of OPBTs correctly, they neglect currents injected at the base electrode, which leads to unrealistically low off-currents and high ON/OFF ratios. Here, a tunneling model is developed that is capable of describing injection of charges through a thin oxide layer formed around the base electrode of OPBTs. With the help of this injection model, the performance of the base-collector diode of OPBTs is discussed. In particular, the model is used to explain the reduction in backward currents due to an exposure to ambient air by an increase in the thickness of the oxide layer. Furthermore, the tunnel model is used to show that the reduction in backward currents of the base-collector diode leads to a decrease in off-currents of complete OPBTs, which in turn leads to an increase in their ON/OFF ratio. 

Abstract Organic electrochemical transistors (OECTs) operate at very low voltages, transduce ions into electronic signals, and reach extremely large transconductance values, making them ideally suited for bio‐sensing applications. However, despite their promising performance, the dependence of their maximum transconductance on device geometry and applied voltages are not correctly captured by current capacitive device models. Here, current scaling laws are revised in the light of a recently developed 2D device model that adequately accounts for drift and diffusion of ions inside the polymer channel. It is shown that the maximum transconductance of the devices is found at the transition between the depletion and accumulation region of the transistors, which as well provides an explanation for the observed shift of the transconductance peak with geometric dimensions and the drain potential. Overall, the results provide a better understanding of the working mechanisms of OECTs, and facilitate design rules to optimize OECT performance further. 

Abstract Phosphate oxyanions play central roles in biological, agricultural, industrial, and ecological processes. Their high hydration energies and dynamic properties present a number of critical challenges limiting the development of sensing technologies that are cost‐effective, selective, sensitive, field‐deployable, and which operate in real‐time within complex aqueous environments. Here, a strategy that enables the fabrication of an electrolyte‐gated organic field‐effect transistor (EGOFET) is demonstrated, which overcomes these challenges and enables sensitive phosphate quantification in challenging aqueous environments such as seawater. The device channel comprises a composite layer incorporating a diketopyrrolopyrrole‐based semiconducting polymer and a π‐conjugated penta‐t‐butylpentacyanopentabenzo[25]annulene “cyanostar” receptor capable of oxyanion recognition and embodies a new concept, where the receptor synergistically enhances the stability and transport characteristics via doping. Upon exposure of the device to phosphate, a current reduction is observed, consistent with dedoping upon analyte binding. Sensing studies demonstrate ultrasensitive and selective phosphate detection within remarkably low limits of detection of 178 × 10⁻¹²m(17.3 parts per trillion) in buffered samples and stable operation in seawater. This receptor‐based doping strategy, in conjunction with the versatility of EGOFETs for miniaturization and monolithic integration, enables manifold opportunities in diagnostics, healthcare, and environmental monitoring.