sensing-barrier-tissue-disruption-with-an-organic-electrochemical

Sensing of Barrier Tissue Disruption with an Organic Electrochemical Transistor

The gastrointestinal tract is an example of barrier tissue that provides a physical barrier against entry of pathogens and toxins, while allowing the ...

Johns Hopkins University

Solution-processable organic semiconductors are central to developing viable printed electronics, and performance comparable to that of amorphous silicon has been reported for films grown from soluble semiconductors. However, the seemingly desirable formation of large crystalline domains introduces grain boundaries, resulting in substantial device-to-device performance variations. Indeed, for films where the grain-boundary structure is random, a few unfavourable grain boundaries may dominate device performance. Here we isolate the effects of molecular-level structure at grain boundaries by engineering the microstructure of the high-performance n-type perylenediimide semiconductor PDI8-CN2 and analyse their consequences for charge transport. A combination of advanced X-ray scattering, first-principles computation and transistor characterization applied to PDI8-CN2 films reveals that grain-boundary orientation modulates carrier mobility by approximately two orders of magnitude. For PDI8-CN2 we show that the molecular packing motif (that is, herringbone versus slip-stacked) plays a decisive part in grain-boundary-induced transport anisotropy. The results of this study provide important guidelines for designing device-optimized molecular semiconductors.

Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films.

Microstructural origin of high mobility in high-performance poly(thieno-thiophene) thin-film transistors.

As thin films become increasingly popular (for solar cells, LEDs, microelectronics, batteries), quantitative morphological and crystallographic information is needed to predict and optimize the film's electrical, optical, and mechanical properties. This quantification can be obtained quickly and easily with X-ray diffraction using an area detector in two sample geometries. In this paper, we describe a methodology for constructing complete pole figures for thin films with fiber texture (isotropic in-plane orientation). We demonstrate this technique on semicrystalline polymer films, self-assembled nanoparticle semiconductor films, and randomly packed metallic nanoparticle films. This method can be immediately implemented to help understand the relationship between film processing and microstructure, enabling the development of better and less expensive electronic and optoelectronic devices.

Quantification of thin film crystallographic orientation using X-ray diffraction with an area detector.

The integration of an organic electrochemical transistor with human barrier tissue cells provides a novel method for assessing toxicology of compounds in vitro. Minute variations in paracellular ionic flux induced by toxic compounds are measured in real time, with unprecedented temporal resolution and extreme sensitivity.

Measurement of barrier tissue integrity with an organic electrochemical transistor.

The gastrointestinal epithelium provides a physical and biochemical barrier to the passage of ions and small molecules; however this barrier may be breached by pathogens and toxins. The effect of individual pathogens/toxins on the intestinal epithelium has been well characterized: they disrupt barrier tissue in a variety of ways, such as by targeting tight junction proteins, or other elements of the junctions between adjacent cells. A variety of methods have been used to characterize disruption in barrier tissue, such as immunofluorescence, permeability assays and electrical measurements of epithelia resistance, but these methods remain time consuming, costly and ill-suited to diagnostics or high throughput toxicology.

Validation of the organic electrochemical transistor for in vitro toxicology.

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.

High transconductance organic electrochemical transistors.

Ion flow across polarized epithelia is a tightly regulated process. Measurement of the transepithelial resistance is a highly relevant parameter for assessing the function or health of the tissue. Dynamic, electrical measurements of transepithelial ion flow are preferred as they provide the most accurate snapshot of effects of external stimuli. Enteric pathogens such as Salmonella typhimurium are known to disrupt ion flow in gastrointestinal epithelia. Here, for the first time, the use of organic transistors as a powerful potential alternative for front-line, disposable, high-throughput diagnostics of enteric pathogens is demonstrated. The transistors' ability to detect early and subtle changes in transepithelial ion flow is capitalized upon to develop a highly sensitive detector of epithelial integrity. Stable operation of the organic devices under physiological conditions is shown, followed by dynamic, pathogen-specific diagnosis of infection of epithelia. Further, operation of the device is possible in complex matrices, showing particular promise for food and safety applications.

Article	Year
Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films. Nature materials\| PubMed ID: 19898460	2009
Microstructural origin of high mobility in high-performance poly(thieno-thiophene) thin-film transistors. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 20217772	2010
Quantification of thin film crystallographic orientation using X-ray diffraction with an area detector. Langmuir : the ACS journal of surfaces and colloids\| PubMed ID: 20361783	2010
Measurement of barrier tissue integrity with an organic electrochemical transistor. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 22949380	2012
Validation of the organic electrochemical transistor for in vitro toxicology. Biochimica et biophysica acta\| PubMed ID: 23246813	2013
High transconductance organic electrochemical transistors. Nature communications\| PubMed ID: 23851620	2013
Dynamic Monitoring of Salmonella typhimurium Infection of Polarized Epithelia Using Organic Transistors. Advanced healthcare materials\| PubMed ID: 24497469	2014

Leslie H. Jimison

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