NANOELECTRONIC DEVICES FOR SENSITIVE DETECTION OF BIOMARKERS IN HEALTHCARE MONITORING

In recent years, biosensors have seen an exponential rise of their applications in a number of fields including the field of health care monitoring, particularly in point-of-care diagnostics. With the contemporary rise of nanotechnology, these biosensors have experienced an ever-growing inclusion of nano scale electronic devices or nanoelectronic devices to exploit the plethora of advantages of nanoelectronics. The performances of these nanoelectronic devices, however, largely depend on the nanomaterials used. Especially, carbon-based nanomaterials such as carbon nanotubes (CNTs) and graphene have proven to be superior candidates compared to others because of their multitude of electronic and mechanical properties suitable for biosensing. In particular, graphene-based FET (GFET) that combines the favorable material properties of graphene as well as the device properties of field-effect transistor have demonstrated its potential in biosensing with high sensitivity and signal-to-noise ratio (SNR). Though GFETs have been applied for sensitive detection of a number of analytes, there are still areas for further development in a number of ways—application of the platform for sensing new biomarkers, developing an integrated microfluidics platform, etc. in order to improve the sensing performances as well as applicability in real-world setting. Therefore, in this seminar, I will discuss the current states and challenges of the GFET-based sensing and present my work to further advance this platform. Moreover, development of a flexible GFET biosensor compatible with wearable platform will also be discussed. To provide the biosensors with the required selectivity, DNA-based aptamers with specific affinity towards the target analyte are used. However, conventional techniques for functionalization of aptamers suffer from several challenges including low throughput, poor control, and long turnaround time. To address these challenges, I will present my efforts on the development of new strategies to address these challenges both on CNT and graphene-based platforms

Materials, Mechanics, and Patterning Techniques for Elastomer-Based Stretchable Conductors

Stretchable electronics represent a new generation of electronics that utilize soft, deformable elastomers as the substrate or matrix instead of the traditional rigid printed circuit boards. As the most essential component of stretchable electronics, the conductors should meet the requirements for both high conductivity and the capability to maintain conductive under large deformations such as bending, twisting, stretching, and compressing. This review summarizes recent progresses in various aspects of this fascinating and challenging area, including materials for supporting elastomers and electrical conductors, unique designs and stretching mechanics, and the subtractive and additive patterning techniques. The applications are discussed along with functional devices based on these conductors. Finally, the review is concluded with the current limitations, challenges, and future directions of stretchable conductors

Technologies for printing sensors and electronics over large flexible substrates: a review

Printing sensors and electronics over flexible substrates is an area of significant interest due to low-cost fabrication and possibility of obtaining multifunctional electronics over large areas. Over the years, a number of printing technologies have been developed to pattern a wide range of electronic materials on diverse substrates. As further expansion of printed technologies is expected in future for sensors and electronics, it is opportune to review the common features, complementarities and the challenges associated with various printing technologies. This paper presents a comprehensive review of various printing technologies, commonly used substrates and electronic materials. Various solution/dry printing and contact/non-contact printing technologies have been assessed on the basis of technological, materials and process related developments in the field. Critical challenges in various printing techniques and potential research directions have been highlighted. Possibilities of merging various printing methodologies have been explored to extend the lab developed standalone systems to high-speed roll-to-roll (R2R) production lines for system level integration

신축성 있고 착용 가능한 탄소 나노튜브 기반 전자 기술

학위논문 (박사) -- 서울대학교 대학원 : 공과대학 협동과정 바이오엔지니어링전공, 2020. 8. 김대형.Networks of carbon nanotubes (CNTs) are a promising candidate for use as a basic building block for next-generation soft electronics, owing to their superior mechanical and electrical properties, chemical stability, and low production cost. In particular, the CNTs, which are produced as a mixture of metallic and semiconducting CNTs via chemical vapor deposition, can be sorted according to their electronic types, which makes them useful for specific purposes: semiconducting CNTs can be employed as channel materials in transistor-based applications and metallic CNTs as electrodes. However, the development of CNT-based electronics for soft applications is still at its infant stage, mainly limited by the lack of solid technologies for developing high-performance deformable devices whose electrical performances are comparable to those fabricated using conventional inorganic materials. In this regard, soft CNT electronics with high mechanical stability and electrical performances have been pursued. First, wearable nonvolatile memory modules and logic gates were fabricated by employing networks of semiconducting CNTs as the channel materials, with strain-tolerant device designs for high mechanical stability. The fabricated devices exhibited low operation voltages, high device-to-device uniformity, on/off ratios, and on-current density, while maintaining its performance during ~30% stretching after being mounted on the human skin. In addition, various functional logic gates verified the fidelity of the reported technology, and successful fabrication of non-volatile memory modules with wearable features has been reported for the first time at the time of publication. Second, the networks of semiconducting CNTs were used to fabricate signal amplifiers with a high gain of ~80, which were then used to amplify electrocardiogram (ECG) signals measured using a wearable sensor. At the same time, color-tunable organic light-emitting diodes (CTOLEDs) were developed based on ultra-thin charge blocking layer that controlled the flow of excitons during different voltage regimes. Together, they were integrated to construct a health monitoring platform whereby real-time ECG signals could be detected while simultaneously notifying its user of the ECG status via color changes of the wearable CTOLEDs. Third, intrinsically stretchable CNT transistors were developed, which was enabled by the developments of thickness controllable, vacuum-deposited stretchable dielectric layer and vacuum-deposited metal thin films. Previous works employed strain-tolerant device designs which are based on the use of filamentary serpentine-shaped interconnections, which severely sacrifice the device density. The developed stretchable dielectric, compatible with the current vacuum-based microfabrication technology, exhibited excellent insulating properties even for nanometer-range thicknesses, thereby enabling significant electrical performance improvements such as low operation voltage and high device uniformity/reproducibility, which has not been realized in the most advanced intrinsically stretchable transistors of today.탄소 나노튜브는 뛰어난 전기적, 화학적, 그리고 기계적 특성을 갖고 있어 차세대 유연 전자소자의 핵심 소재 중 하나로 각광을 받고 있으나, 아직까지 이를 이용한 실용적인 유연 전자소자의 개발은 실현되지 않고 있다. 이는 탄소 나노튜브의 전기적 특성대로 완벽히 분류해 낼 수 있는 기술, 탄소 나노튜브를 소자의 원하는 위치에 정확히 원하는 양만큼 네트워크 형태 혹은 정렬된 형태로 증착하는 기술, 그리고 유연 전자소자를 구성하는 다른 물질들의 개발 기술의 부재 때문이다. 지난 10여년간 해당 기술들은 광범위하게 연구되어지고 있으나, 탄소 나노튜브를 활용한 우수한 유연 전자소자 개발을 위한 핵심 기술들의 발전은 아직 초기 단계에 있다. 따라서 이 논문을 통해 탄소 나노튜브를 유연 전자소자에 적용시킬 수 있는 새로운 기술을 소개하고자 한다. 첫번째로 탄소 나노튜브와 유연 전자소자의 소자 디자인을 이용하여 피부위에 증착 가능한 비휘발성 메모리 소자를 제작하였고, 해당 기술을 이용하여 피부위에서 안전하게 동작할 수 있는 다양한 기초 회로들을 구현하였다. 탄소 나노튜브 기반 메모리 전자 소자 및 회로는 다양한 외부 응력이 가해져도 안정적으로 동작을 하였고, 개발된 기술을 통해 보다 실용적인 탄소 나노튜브 기반 유연 전자 소자의 제작 조건을 확립할 수 있었다. 두번째로 위에 개발된 기술을 바탕으로, 보다 복잡한 탄소 나노튜브 기반 유연 회로 및 구동전압에 따라 발광색이 변환하는 색변환 소자를 제작하여 해당 소자들이 피부위에 부착되어 잘 작동되도록 구현하였다. 그리고 이 두 가지 웨어러블 전자소자를 통합하여 실시간으로 심전도를 측정하여 탄소 나노튜브 기반 전자소자를 통해 해당 신호를 증폭시키고, 신호의 상태를 색변환 소자로 나타낼 수 있는 심전도 모니터 시스템을 구현하였다. 세번째로 진공 증착이 가능한 유연 절연체를 개발하여, 기존의 유연 전자소자들이 가지고 있던 극명한 한계를 극복하였다 (높은 구동 전압, 낮은 집적도, 대면적 소자 선능 균일도 등). 기존의 액상 기반 증착을 위주로 한 유연 전자 소자들은 무기물질 기반 전자소자 대비 극심한 성능 저하를 보여주었는데, 이를 해결하기 위해 새로운 절연물질을 개발하고 탄소 나노튜브 기반 유연 전자소자에 적용하여 그 가능성을 보여주었다.Chapter 1. Introduction 1 1.1 Discovery of CNTs and their benefits for soft electronic applications 1 1.2 Electrical sorting of CNTs 5 1.3 Deposition methods of solution-processed semiconducting CNTs 7 1.4 Conclusion 23 1.5 References 24 Chapter 2. Stretchable Carbon Nanotube Charge-Trap Floating-Gate Memory and Logic Devices for Wearable Electronics 32 2.1 Introduction 32 2.2 Experimental section 34 2.3 Results and discussion 36 2.4 Conclusion 62 2.5 References 63 Chapter 3. Wearable Electrocardiogram Monitor Using Carbon Nanotube Electronics and Color-Tunable Organic Light-Emitting Diodes 67 3.1 Introduction 67 3.2 Experimental section 70 3.3 Results and discussion 73 3.4 Conclusion 97 3.5 References 98 Chapter 4. Medium-Scale Electronic Skin Based on Carbon Nanotube Transistors with Vacuum-Deposited Stretchable Dielectric Film 102 4.1 Introduction 102 4.2 Experimental section 106 4.3 Result and discussion 111 4.4 Conclusion 135 4.5 References 136Docto

Flexible and Stretchable Electronics

Flexible and stretchable electronics are receiving tremendous attention as future electronics due to their flexibility and light weight, especially as applications in wearable electronics. Flexible electronics are usually fabricated on heat sensitive flexible substrates such as plastic, fabric or even paper, while stretchable electronics are usually fabricated from an elastomeric substrate to survive large deformation in their practical application. Therefore, successful fabrication of flexible electronics needs low temperature processable novel materials and a particular processing development because traditional materials and processes are not compatible with flexible/stretchable electronics. Huge technical challenges and opportunities surround these dramatic changes from the perspective of new material design and processing, new fabrication techniques, large deformation mechanics, new application development and so on. Here, we invited talented researchers to join us in this new vital field that holds the potential to reshape our future life, by contributing their words of wisdom from their particular perspective

Recent Advances in Printed Capacitive Sensors

In this review paper, we summarize the latest advances in the field of capacitive sensors fabricated by printing techniques. We first explain the main technologies used in printed electronics, pointing out their features and uses, and discuss their advantages and drawbacks. Then, we review the main types of capacitive sensors manufactured with different materials and techniques from physical to chemical detection, detailing the main substrates and additives utilized, as well as the measured ranges. The paper concludes with a short notice on status and perspectives in the field.H2020-MSCA-IF-2017-794885-SELFSEN

Layer by layer printing of nanomaterials for large-area, flexible electronics

Large-area electronics, including printable and flexible electronics, is an emerging concept which aims to develop electronic components in a cheaper and faster manner, especially on those non-conventional substrates. Being flexible and deformable, this new form of electronics is regarded to hold great promises for various futuristic applications including the internet of things, virtual reality, healthcare monitoring, prosthetics and robotics. However, at present, large-area electronics is still nowhere near the commercialisation stage, which is due to several problems associated with performance, uniformity and reliability, etc. Moreover, although the device’s density is not the major concern in printed electronics, there is still a merit in further increasing the total number of devices in a limited area, in order to achieve more electronic blocks, higher performance and multiple functionalities. In this context, this Ph.D. thesis focuses on the printing of various nanomaterials for the realisation of high-performance, flexible and large-area electronics. Several aspects have been covered in this thesis, including the printing dynamics of quasi-1D NWs, the contact problem in device realisation and the strategy to achieve sequential integration (3D integration) of the as-printed devices, both on rigid and flexible substrates. Promisingly, some of the devices based on the printed nanomaterial show a comparable performance to the state-of-the-art technology. With the demonstrated 3D integration strategy, a highly dense array of electronic devices can be potentially achieved by printing method. This thesis also touches on the problem associated with the circuit and system realisation. Specifically, graphene-based logic gates and NW based UV sensing circuit has been discussed, which shows the promising applications of nanomaterial-based electronics. Future work will be focusing on extending the UV sensing circuit to an active matrix sensor array

Technological Integration in Printed Electronics

Conventional electronics requires the use of numerous deposition techniques (e.g. chemical vapor deposition, physical vapor deposition, and photolithography) with demanding conditions like ultra-high vacuum, elevated temperature and clean room facilities. In the last decades, printed electronics (PE) has proved the use of standard printing techniques to develop electronic devices with new features such as, large area fabrication, mechanical flexibility, environmental friendliness and—potentially—cost effectiveness. This kind of devices is especially interesting for the popular concept of the Internet of Things (IoT), in which the number of employed electronic devices increases massively. Because of this trend, the cost and environmental impact are gradually becoming a substantial issue. One of the main technological barriers to overcome for PE to be a real competitor in this context, however, is the integration of these non-conventional techniques between each other and the embedding of these devices in standard electronics. This chapter summarizes the advances made in this direction, focusing on the use of different techniques in one process flow and the integration of printed electronics with conventional systems

Chitosan gated organic transistors printed on ethyl cellulose as a versatile platform for edible electronics and bioelectronics

Edible electronics is an emerging research field targeting electronic devices that can be safely ingested and directly digested or metabolized by the human body. As such, it paves the way to a whole new family of applications, ranging from ingestible medical devices and biosensors, to smart labelling for food quality monitoring and anti-counterfeiting. Being a newborn research field, many challenges need to be addressed to realize fully edible electronic components. In particular, an extended library of edible electronic materials is required, with suitable electronic properties depending on the target device and compatible with large-area printing processes, to allow scalable and cost-effective manufacturing. In this work, we propose a platform for future low-voltage edible transistors and circuits that comprises an edible chitosan gating medium and inkjet printed inert gold electrodes, compatible with low thermal budget edible substrates, such as ethylcellulose. We report the compatibility of the platform, characterized by critical channel features as low as 10 µm, with different inkjet printed carbon-based semiconductors, including biocompatible polymers present in the picograms range per device. A complementary organic inverter is also demonstrated with the same platform as a proof-of-principle logic gate. The presented results offer a promising approach to future low-voltage edible active circuitry, as well as a testbed for non-toxic printable semiconductors

Laajan pinta-alan elektroniikan valmistusmenetelmiä

In Large Area Electronics (LAE) there are multiple processing methods to take advantage of. Components can be produced for example by directly printing patterned layers on top of each other. Most common printing methods are gravure, flexographic, silk screen and inkjet. Electronics done only by such processes suffer from the limitations stated by the printable materials and the process equipment. This thesis shows some critical LAE processing challenges, and introduces new ways to overcome them. The goal is to use roll-to-roll compatible methods. Some traditional processing techniques are used in a new way. Commercial and prototype materials are used in the testing. The work includes experimental results of printed thin films made with polymer or carbon nanotube semiconductors and either low- or high permittivity dielectrics. After material selection, the transistor electrode quality and pattern resolution (dimensions) govern the electrical performance. Electrical results of low-voltage (5V) thin film transistors and circuits are reported. This work includes the experimental results of roll-to-roll (R2R) compatible thin metal film patterning methods like etching with a new printable gel etchant, and high resolution laser ablation. Furthermore, a new lamination concept is introduced. Laminating together two separate substrates allows new possible material combinations and new electrode options for both sides of the device. Finally, these methods are combined in a demonstration device: a tactile sensor matrix is built using air-gap transistors. The transistors are constructed using R2R printed active layers including gel etched electrodes on one foil, and inkjet printed spacers and electrodes on another foil. When foils are laminated together, air-gap transistors are formed, and the flexible structure make the transistors sensitive to tactile input. The shape and sensitivity of such sensor structure is easy to modify for different applications.Laajan pinta-alan elektroniikan tuotantoon on useita mahdollisia menetelmiä. Yksinkertaisimmillaan prosessointi on additiivista; siinä elektroniikan komponentti toteutetaan kerros kerrokselta, esimerkiksi kuvioiduilla painoprosesseilla. Yleisimmät alan painomenetelmät ovat syväpaino, fleksografinen paino, silkkipaino ja mustesuihkutulostus. Tällä tavoin tuotetut komponentit eivät yleensä ole suorituskyvyltään riittäviä todellisiin sovelluksiin, johtuen painotekniikan ja painettavien materiaalien rajoituksista. Tämän vuoksi laajan pinta-alan elektroniikassa on usein mukana myös muilla tuotantoprosesseilla toteutettuja kerroksia tai pintakäsittelyjä. Tässä työssä esitetään keinoja laajan pinta-alan elektroniikan suorituskyvyn parantamiseksi käyttäen perinteisiä menetelmiä uudella tavalla. Tavoitteena on rullalta-rullalle (R2R) yhteensopiva prosessi. Tutkimukseen on käytetty sekä kaupallisia, että kehitysasteella olevia materiaaleja. Kokeellisessa työssä on tutkittu pienen ja suuren permittiivisyyden hilaeristekerroksia, ja polymeeri- ja hiilinanoputki-puolijohteita ohutkalvotransistoreissa. Materiaalin valinnan jälkeen komponenttien dimensiot ja kuvioinnin laatu määrittävät suorituskyvyn. Ohuilla kerroksilla saatiin aikaan suhteellisen matalalla (5V) käyttöjännitteellä toimivia transistoreja ja piirejä. Tässä työssä esitetään painoprosessiin soveltuva ohuen metallikerroksen etsausmenetelmä, sekä hienokuviointiin kykenevä laser-kuviointimenetelmä. Työssä esitetään myös erityinen laminointimenetelmä. Se mahdollistaa tarkasti kuvioidut elektrodit rakenteen kummallakin puolella, sekä materiaalit jotka eivät ole muuten painettavissa tai prosessoitavissa päällekkäin. Tämä tuottaa kahden substraatin väliin luontaisesti suojaan prosessoidun rakenteen. Lopuksi esitetään esimerkkinä kosketussensorisovellus, jossa yhdistetään R2R massaprosessoitu transistorirakenne, mustesuihkutulostettu erottava välirakenne ja laminointimenetelmä. Sensorin muoto ja herkkyysalue ovat vapaasti muokattavissa eri käyttötarkoituksiin sopivaksi