Eleni Stavrinidou

High transconductance organic electrochemical transistors.

The development of transistors with high gain is essential for applications ranging from switching elements and drivers to transducers for chemical and biological sensing. Organic transistors have become well-established based on their distinct advantages, including ease of fabrication, synthetic freedom for chemical functionalization, and the ability to take on unique form factors. These devices, however, are largely viewed as belonging to the low-end of the performance spectrum. Here we present organic electrochemical transistors with a transconductance in the mS range, outperforming transistors from both traditional and emerging semiconductors. The transconductance of these devices remains fairly constant from DC up to a frequency of the order of 1 kHz, a value determined by the process of ion transport between the electrolyte and the channel. These devices, which continue to work even after being crumpled, are predicted to be highly relevant as transducers in biosensing applications.

Direct measurement of ion mobility in a conducting polymer.

Using planar junctions between the conducting polymer PEDOT:PSS and various electrolytes, it is possible to inject common ions and directly observe their transit through the film. The 1D geometry of the experiment allows a straightforward estimate of the ion drift mobilities.

High speed and high density organic electrochemical transistor arrays

A generic lithographic process is presented that allows the fabrication of high density organic electrochemical transistor arrays meant to interface with aqueous electrolytes. The channels of the transistors, which were 6 μm long, were made of the conducting polymer poly(3,4-ethylenedioxythiophene) doped with poly(styrene sulfonate) and were in direct contact with phosphate buffered saline. Source and drain electrodes and interconnects were insulated by parylene C, a biocompatible material. The transistors operated at low voltages and showed a response time of the order of 100 μs.

PEDOT: gelatin composites mediate brain endothelial cell adhesion

Conducting polymers (CPs) are increasingly being used to interface with cells for applications in both bioelectronics and tissue engineering. To facilitate this interaction, cells need to adhere and grow on the CP surface. Extracellular matrix components are usually necessary to support or enhance cell attachment and growth on polymer substrates. Here we show the preparation of PEDOT(TOS):gelatin composites as a new biocompatible substrate for use in tissue engineering. Gelatin, a derivative of the extracellular matrix protein collagen, was incorporated into poly(3,4 ethylenedioxythiophene)-tosylate (PEDOT(TOS)) films via vapour phase polymerisation (VPP) without changing the electrochemical properties of the CP. Further, gelatin, incorporated into the PEDOT(TOS) film, was found to specifically support bovine brain capillary endothelial cell adhesion and growth, indicating that the functionality of the biomolecule was maintained. The biocompatibility of the composite films was demonstrated indicating the significant future potential of biocomposites of this type for use in promoting cell adhesion in electrically active materials for tissue engineering.

A facile biofunctionalisation route for solution processable conducting polymer devices

For the majority of biosensors or biomedical devices, immobilization of the biorecognition element is a critical step for device function. To achieve longer lifetime devices and controllable functionalization, covalent immobilisation techniques are preferred over passive adhesion and electrostatic interactions. The rapidly emerging field of organic bioelectronics uses conducting polymers (or small molecules) as the active materials for transduction of the biological signal to an electronic one. While a number of techniques have been utilized to entrap or functionalize conducting polymers deposited by electro- or vapor phase polymerization, covalent functionalization of solution processed films, essential for realizing low cost or high throughput fabrication, has not been thoroughly investigated. In this study we show a versatile biofunctionalization technique for the solution processable conducting polymer poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate) PEDOT:PSS, which is a commercially available material, and has a record high conductivity. Addition of poly(vinyl alcohol) (PVA) into the solution with PEDOT:PSS provides a handle for subsequent silanization with a well-characterised silane reagent, allowing for covalent linkage of biological moieties onto PEDOT:PSS films. We show homogenous and large-scale biofunctionalization with polypeptides and proteins, as well as maintenance of the biological functionalities of the proteins. In addition, no deleterious effects are noted on the electronic or ionic transport properties of the conducting polymer films due to incorporation of the PVA.

A simple model for ion injection and transport in conducting polymers

We present a simple analytical model that describes ion transport in a planar junction between an electrolyte and a conducting polymer film. When ions are injected in the film, holes recede, leading to partial dedoping of the film. This is modeled by two resistors in series, an ionic one for the dedoped part and an electronic one for the still-doped part. We show that analytical predictions can be made for the temporal evolution of the drift length of ions and the current, variables that could be assessed experimentally. A numerical model based on forward time iteration of drift/diffusion equations is used to validate these predictions. Using realistic materials parameters, we find that the analytical model can be used to obtain the ion drift mobility in the film, and as such, it might be useful towards the development of structure vs. ion transport properties relationships in this important class of electronic materials.

In vivo polymerization and manufacturing of wires and supercapacitors in plants

Significance Plants with integrated electronics, e-Plants, have been presented recently. Up to now the devices and circuits have been manufactured in localized regions of the plant due to limited distribution of the organic electronic material. Here we demonstrate the synthesis and application of a conjugated oligomer that can be delivered in every part of the vascular tissue of a plant and cross through the veins into the apoplast of leaves. The oligomer polymerizes in vivo due to the physicochemical environment of the plant. We demonstrate long-range conducting wires and supercapacitors along the stem. Our findings open pathways for autonomous energy systems, distributed electronics, and new e-Plant device concepts manufactured in living plants. Electronic plants, e-Plants, are an organic bioelectronic platform that allows electronic interfacing with plants. Recently we have demonstrated plants with augmented electronic functionality. Using the vascular system and organs of a plant, we manufactured organic electronic devices and circuits in vivo, leveraging the internal structure and physiology of the plant as the template, and an integral part of the devices. However, this electronic functionality was only achieved in localized regions, whereas new electronic materials that could be distributed to every part of the plant would provide versatility in device and circuit fabrication and create possibilities for new device concepts. Here we report the synthesis of such a conjugated oligomer that can be distributed and form longer oligomers and polymer in every part of the xylem vascular tissue of a Rosa floribunda cutting, forming long-range conducting wires. The plant’s structure acts as a physical template, whereas the plant’s biochemical response mechanism acts as the catalyst for polymerization. In addition, the oligomer can cross through the veins and enter the apoplastic space in the leaves. Finally, using the plant’s natural architecture we manufacture supercapacitors along the stem. Our results are preludes to autonomous energy systems integrated within plants and distribute interconnected sensor–actuator systems for plant control and optimization.

Engineering hydrophilic conducting composites with enhanced ion mobility

Ion mobility has a direct influence on the performance of conducting polymers in a number of applications as it dictates the operational speed of the devices. We report here the enhanced ion mobility of poly(3,4-ethylene dioxythiophene) after incorporation of gelatin. The gelatin-rich domains were seen to provide an ion pathway through the composites.

A physical interpretation of impedance at conducting polymer/electrolyte junctions

We monitor the process of dedoping in a planar junction between an electrolyte and a conducting polymer using electrochemical impedance spectroscopy performed during moving front measurements. The impedance spectra are consistent with an equivalent circuit of a time varying resistor in parallel with a capacitor. We show that the resistor corresponds to ion transport in the dedoped region of the film, and can be quantitatively described using ion density and drift mobility obtained from the moving front measurements. The capacitor, on the other hand, does not depend on time and is associated with charge separation at the moving front. This work offers a physical description of the impedance of conducting polymer/electrolyte interfaces based on materials parameters.

Highly porous scaffolds of PEDOT:PSS for bone tissue engineering

Graphical abstract