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A Complete Interfacial System Solution for Liquid Metal Electronics

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A Complete Interfacial System Solution for Liquid Metal Electronics A Complete Interfacial System Solution for Liquid Metal Electronics A dissertation submitted to the Graduate School of the University of Cincinnati in partial fulfillment of the requirements for the degree of Doctor of Philosophy in the Department of Materials Science & Engineering of the College of Engineering & Applied Science by Sarah E. Holcomb B.S., Rensselaer Polytechnic Institute, 2013 Committee Chair: Jason C. Heikenfeld, Ph.D. Abstract Liquid metal electronic devices have numerous advantages over traditional solid devices such as the ability to be flexed and stretched or reconfigured. Examples of such devices are wires, switches, polarizers, and antennas. Previously, mercury has been used as the room temperature liquid metal of choice but has been recently replaced by gallium liquid metal alloys (GaLMAs) which are non-toxic, have extremely low vapor pressures, and can remain liquid at temperatures as low as -19°C. A key difference in the performance of GaLMAs vs. mercury is the mechanically stabilizing, passivating oxide which forms instantly on the surface of GaLMAs in as little as 1 ppm oxygen environments. This oxide presents a significant challenge for reconfigurable device applications because it “sticks” to most surfaces, preventing reversible shape change, which alters the desired electrical performance. Proposed here are two novel methods of overcoming this challenge. These methods enable new capabilities for reconfigurable electronic devices. The first approach involves removing the oxide in situ as it is continuously formed in all practically achievable device environments. Oxide removal is commonly done through the use of hydrochloric acid (aqueous or vapor), which reacts with the gallium oxide to produce gallium chloride, which is not mechanically stabilizing, and water. The water produced from this reaction can have detrimental effects for interface-sensitive methods of actuation, one example is electrowetting. Furthermore, surrounding the GaLMA in a conductive environment diminishes the performance capabilities of the device. Combining HCl with an insulating and hygroscopic environment, such as silicone oil, allows for the GaLMA to retain its fluidic properties of shape change without sticking while not interfering with the electrical performance of the device. Importantly, the water produced at the interface diffuses into the bulk of the oil solution where it has a negligible effect on the system. The second approach utilizes the oxide to modify and tune the surface properties of the liquid metal. Phosphonic acids (PAs) bind strongly to metal oxide to form monolayers and have been used on transparent metal oxides to tune surface properties for applications such as organic solar cells. More recently, this approach has also been applied to prevent sticking or alloying of GaLMAs to other metals. Because there are not competing reactions, controlling the GaLMA interface by modifying the native oxide yields a more stable system than removing the oxide. Copyright Page Acknowledgements First and foremost, I would like to express my sincerest gratitude to my advisors, Dr. Jason Heikenfeld and Dr. Christopher Tabor, for their invaluable advice and guidance on both academic and personal levels. Without their encouragement and knowledge to support me throughout this thesis, my Ph.D. would have never been as productive and efficient. I would also like to thank my doctoral dissertation committee, Dr. Ashley Paz y Puente, Dr. Dale Schaefer and Dr. Je-Hyeong Bahk, for their time and their inspiring suggestions. I owe my deepest appreciation to Dr. David Mast and Dr. Michael Dickey (NCSU) for technical discussions and sharing with me their expertise. I would also like to give special thanks to Dr. Michael Brothers (AFRL) for his precious help with chemical characterization and Dr. Alex Cook (AFRL) for help with electrical measurements and automating test setups. I am heartily grateful to Aaron Diebold for his collaborations in electrowetting experiments and device design/testing. I would like to extend my gratitude to the staffs of the Department of Electronics and Computing Systems and of the Department of Mechanical and Materials Engineering, especially Tony Seta, for all their help. I wish to thank my colleagues of the Novel Devices Laboratory and Air Force Research Laboratory for the memorable discussions and all the help. This journey would not have been as fun and enjoyable without all of you. I would like to express a special thanks to my husband, Sean, for his continued and unfailing love, support and understanding during the pursuit of my Ph.D. You were always around at times I thought that it is impossible to continue and you helped me to keep things in perspective. Finally, I would like to dedicate this work to my parents who have inspired me in life as well as in pursuing higher education. I greatly value their contribution and deeply appreciate their belief in me. Table of Contents Abstract ........................................................................................................................................................ ii Copyright Page ........................................................................................................................................... iv Acknowledgements .................................................................................................................................... v Table of Contents ....................................................................................................................................... vi List of Figures .......................................................................................................................................... viii Chapter 1: Introduction .............................................................................................................................. 1 1.1 Introduction ......................................................................................................................................... 1 1.2 Research Aims and Outline ................................................................................................................ 2 Chapter 2: Literature Review ..................................................................................................................... 5 2.1 Introduction ......................................................................................................................................... 5 2.2 Key Challenges .................................................................................................................................. 6 2.3 Gallium Liquid Metal Alloys ................................................................................................................ 7 2.4 Oxide Characteristics ......................................................................................................................... 8 2.4.1 Mechanical Properties .............................................................................................................. 8 2.4.2 Electrical Properties ................................................................................................................ 11 2.4.3 Structure ................................................................................................................................. 11 2.5 Oxide Removal Methods .................................................................................................................. 14 2.5.1 Chemical ................................................................................................................................. 14 2.5.2 Electrochemical ...................................................................................................................... 16 2.6 Electrical Contacts ............................................................................................................................ 18 2.6.1 Importance of Reliable Electrical Contacts ............................................................................. 18 2.6.2 Chemical Interactions ............................................................................................................. 18 2.6.3 Physical Interactions ............................................................................................................... 20 2.6.4 Electrical Interactions ............................................................................................................. 22 2.7 Conclusions ...................................................................................................................................... 22 2.8 Objective of Research ...................................................................................................................... 23 2.9 References ....................................................................................................................................... 24 Chapter 3: Oxide-Free Actuation of Gallium Liquid Metal Alloys Enabled by Novel Acidified Siloxane Oils .............................................................................................................................................. 27 3.1 Introduction ....................................................................................................................................... 27 3.2 Experimental Materials and Methods ............................................................................................... 30 3.2.1 Synthesis of Acidic
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