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Fabrication and Optimization of Organic FET and Organic Electrolyte Gated FET

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Fabrication and Optimization of Organic FET and Organic Electrolyte Gated FET Fabrication and Optimization of Organic FET and Organic Electrolyte Gated FET Devices for Application as Label-free Biosensors By Roslyn Simone Massey A thesis submitted to the Graduate Program in Electrical & Computer Engineering in conformity with the requirements for the Degree of Master of Applied Science Queen’s University Kingston, Ontario, Canada September, 2019 Copyright © Roslyn Simone Massey, 2019 Abstract Organic Thin-Film Transistors are carbon-based semiconductor devices. Their simple fabrication makes them an ideal candidate for disposable, wearable technologies; an implementation being aptamer- based biosensors. This project produces organic semiconductor aptamer-based biosensors for quantifying biomolecules in synthetic samples mimicking bio-fluids. There are two main effects in a field effect transistor; capacitance and resistance. The semiconductor between the source-drain electrodes is a transient resistor. Capacitance is created by voltage differences across the gate dielectric insulator. Charge buildup at the semiconductor-insulator interface induces a conducting channel through the semiconductor. Channel current can be increased by modulating the source-gate voltage until the current saturation point is reached. The transconductance, ratio of voltage to current change, is device-specific and based on resistance and capacitance. Electrolyte media incorporated within the OFET framework as part of the gate dielectric permits label- free analyte sensing. The liquid-sample/solid-dielectric interface has an electric double layer capacitive effect that alters with biomolecule concentration change, causing the OFETs to experience transconductance change. These sensor devices were fabricated using simple, low-temperature processes. The semiconductor and dielectric stacks were spun on the source-drain electrodes to form the bottom surface, and the top gate was an in-house designed conductive polymer bilayer with a thin PMMA layer then functionalized with aptamers, DNA oligomers that specifically interact with a certain biomolecule. This produces label-free sensors with highly correlated current modulation due to changes in device transconductance. The characterized devices were used to create current vs concentration curves for biomolecule solutions of known concentration. The generated response curves were used to directly correlate device output current to biomolecule concentration. ii The extensive material and processing optimization work conducted in the thesis yielded several performance outcomes comparable to high fabrication requirement OFETS, such as charge mobilities of ~ 0.1 – 0.2 cm2/V-s. The OFET on/off ratios is 1.3x104. The OEGFET device detects 1-2 orders of magnitude change in dosage with a limit of detection of 0.01 µM. An OFET device optimized with a novel dielectric stack demonstrated significant improvements in operating parameters and shelf life. iii Co-Authorship The body of scientific content presented in this work has been developed by the Organic Semiconductor Lab at Queen’s in 2017-18 and Organic Sensors and Devices Lab at Carleton in 2018-19, and through association with Carleton and Queen’s professors is presented in one published conference paper, one submitted manuscript and one manuscript in progress [Authorship references 1-3]. The published conference paper demonstrates the functionality of the fabricated label-free OEGFET transistors for sensing ultrafine concentrations of dopamine in synthetic bio-fluids. The transistors are capable of detecting dopamine in physiologically-relevant concentrations with specificity to the analyte in question. This paper shows that the low-cost transistor is possible. The first submitted manuscript describes a novel composite dielectric that not only increases charge mobility and on/off ratio dramatically, but also increases the shelf life of OFETs from days to months. The final manuscript in progress details the investigation of various OFET device configurations for biosensor applications. It establishes the specificity and reliability of the designed label-free OEGFET sensors and describes the development of a device for implementing the label-free OEGFET sensor. The manuscript also describes novel dielectric stacks proposed for increasing the electrical characteristics of the label-free OEGFET sensors and their production on flexible plastic substrates. The experimental work presented in this dissertation and authorship references 1 and 3 was carried out collaboratively by the author of this dissertation, research supervisor Professor Ravi Prakash, and the organic sensors and devices laboratory at Carleton University, Dr. Siziwe Bebe and Ivan Amor, with aptamers provided by Dr. Maria De Rosa of Carleton University. The electrode patterning was carried out by the author, with semiconductor and dielectric deposition carried out by the author and Dr. Siziwe Bebe. The development of those techniques was a collaboration between the author, her supervisor and Dr. Siziwe Bebe. The sol-gel composite film deposition process was adopted for OFET device from iv reference 3 the from Profs. Freundorfer and Sayer. The experimental data collection was performed by the author, her supervisor, and the Organic Sensors and Devices laboratory at Carleton university. Authorship References: [1] Massey, R; Morin, E; DeRosa, M; Prakash, R; “Label-Free Detection of Dopamine Using Aptamer Enhanced Organic-Electrolyte Gated FET Sensor,” Proc. IEEE International Conference on Flexible and Printable Sensors and systems, Glasgow, 2019, p28. [2] Massey, R; Freundorfer, A; Sayer,M; Prakash, R;. “Thin Film Organic Transistors based on Barium Strontium Titanate Sol-Gel Composite/PMMA Dielectrics”. Organic Electronic Journal, ‘Under Review’, July 2019. [3] Massey, R; Bebe,S; DeRosa, M; Prakash, R. “Ultrasensitive, Label-Free Detection of Cortisol Using Aptamer Enhanced Organic-Electrolyte Gated FET Sensor”. ‘Manuscript in Preparation’, Biosensors and Bioelectronics, August 2019. v Acknowledgements This project was made possible by the involvement of a community of invaluable researchers at Queen’s and Carleton Universities. First, I would like to thank my supervisors, Prof. Ravi Prakash and Prof. Evelyn Morin, for their guidance throughout this research project. This work would not have been possible without their dedication to my academic development and involvement with my day-to-day research. I am grateful for the opportunities already given, and I’m excited to continue the research in coming projects. Likewise, I would like to thank the members of the Organic Sensors and Devices Lab at Carleton University for being part of the work and helping with data collection and sample preparation tasks. In particular, I would like to acknowledge Dr. Siziwe Bebe and Mr. Ivan Amor at Carleton University for all of their vital input on data collection and substrate preparation. I would like to thank Prof. DeRosa of the Ladder group at Carleton for collaborating on the OEGFET biorecognition molecules and making the sensors possible. I would like to thank Prof. Freundorfer and Prof. Sayer for collaborating on a portion of this work. The time and effort spent has opened a new and exciting avenue for further exploration and added impact to this work. I am grateful to the Canadian Microelectronics Corporation for their aid through two financial assistance grants. At the CMC Nanofab Kingston I would like to thank Graham Gibson and Rob Dumont for their instruction on nanofabrication procedures. I am also grateful to the National Science and Engineering Research Council (NSERC) for the Discovery Grant received by Prof. Prakash. vi On a personal note I would like to thank my wonderful partner James Bell and the Massey clan (Mum, Dad, Shona, Johnny and, last but not least, Isla) for the enthusiasm over my work and unconditional support. Thankyou for all the motivation, it made the journey possible. vii Table of Contents Chapter 1 Introduction .................................................................................................................................. 1 1.1 History of Organic Transistors ....................................................................................................... 1 1.1.1 Beginnings ............................................................................................................................. 1 1.1.2 The First Commercial Transistor ........................................................................................... 2 1.1.3 Field Effect Transistor Resurgence ........................................................................................ 2 1.1.4 The First TFT .......................................................................................................................... 3 1.1.5 Enter the Organics ................................................................................................................ 4 1.1.6 Use of TFTs with Organic Transistors .................................................................................... 7 1.1.7 The First OTFTs .................................................................................................................... 10 1.2 Motivation ................................................................................................................................... 12 Chapter 2 Literature Review ....................................................................................................................... 14 2.1 Device Architecture ....................................................................................................................
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