Author Biography

Omar Azzaroni is an Adjunct Professor of Physical Chemistry at the Universidad Nacional de La Plata, Argentina. He is currently a fellow of the Argentinian National Scientific and Technical Research Council (CONICET) and head of the Soft Matter Laboratory at the Universidad Nacional de La Plata. Wolfgang Knoll is an Honorary Professor at the Danube Private University in Krems, Austria. Previously, he was Scientific Managing Director of the Austrian Institute of Technology in Vienna, Austria, and before that one of the Directors at the MPI for Polymer Research in Mainz, Germany

Table of Contents

Foreword xv Preface xvii 1 2D Electronic Circuits for Sensing Applications 1
Diogo Baptista, Ivo Colmiais, Vitor Silva, Pedro Alpuim, and Paulo M. Mendes 1.1 Introduction 1 1.2 Graphene Inductors 3 1.2.1 Modeling of Graphene Inductors 4 1.3 Graphene Capacitors 5 1.3.1 Modeling Graphene Capacitors 8 1.4 2D Material Transistors 9 1.4.1 Most Common Topologies for Transistors 10 1.4.2 Modeling of 2D Materials-Based Transistors 11 1.5 2D Material Diodes 15 1.5.1 Most Common Topologies 16 1.5.2 Modeling of 2D Materials-Based Diodes 17 1.6 Graphene Devices 18 1.6.1 Graphene Frequency Multipliers 18 1.6.2 Graphene Mixers 18 1.6.3 Graphene Oscillators 19 1.6.3.1 Ring Oscillators 19 1.6.3.2 LC Tank Oscillators 19 1.7 Conclusion 19 References 20 2 Large Graphene Oxide for Sensing Applications 25
Jingfeng Huang, J. Amanda Ong, and I.Y. Alfred Tok 2.1 Graphene Oxide (GO) 25 2.2 GO as Biosensors 25 2.3 Large GO 26 2.4 Mechanism of Large GO via Modified Hummers Method 27 2.5 Large GO (Modified Hummers Method) Biosensors 28 2.6 Mechanism of Large GO via Reduced GO Growth 29 2.7 Large GO (Reduced GO Growth) Biosensors 34 2.8 Conclusion 38 2.9 Further Developments 38 References 39 3 Solution-Gated Reduced Graphene Oxide FETs: Device Fabrication and Biosensors Applications 43
Nirton C. S. Vieira, Bianca C. S. Ribeiro, Rodrigo V. Blasques, Bruno C. Janegitz, Fabrício A. dos Santos, and Valtencir Zucolotto 3.1 Introduction 43 3.2 Graphene, Graphene Oxide, and Reduced Graphene Oxide 45 3.2.1 Chemical Reduction 48 3.2.2 Thermal Reduction 49 3.2.3 Electrochemical Reduction 51 3.3 rGO-Based Solution-Gated FETs 52 3.3.1 Manufacturing Strategies 53 3.4 Applications of rGO SG-FETs as Biosensors 57 3.4.1 rGO Functionalization 59 3.4.2 Enzymatic Biosensors 60 3.4.3 Affinity Biosensors 61 3.4.4 Debye Length Screening and How to Overcome It 63 3.5 Final Remarks and Challenges 64 Acknowledgments 65 References 65 4 Graphene-Based Electronic Biosensors for Disease Diagnostics 71
Ahmar Hasnain and Alexey Tarasov 4.1 Introduction 71 4.1.1 A Promise for Diagnostics 71 4.1.2 Principle of Graphene FET Sensor 72 4.2 Device Fabrication Process 75 4.2.1 Graphene Synthesis 75 4.2.2 Graphene Transfer Over Substrates 76 4.2.3 Fabrication of GFET 77 4.2.4 New Developments 78 4.3 Functionalization and Passivation 78 4.3.1 Probe Molecules 79 4.3.2 Immobilization of Probe Molecules 80 4.3.3 Debye Length 81 4.3.4 Passivation 82 4.4 CVD GFETs for Diagnostics 83 4.4.1 Graphene-Based FET Biosensors for Nucleic Acids 83 4.4.2 Graphene-Based FET Biosensors for Antibody–Antigen Interactions 85 4.4.3 Graphene-Based FET Biosensors for Enzymatic Biosensors 87 4.4.4 Graphene-Based FET Biosensors for Sensing of Small Ions 90 4.5 Discussion 92 4.5.1 Summary 92 4.5.2 Challenges 92 4.5.3 Future Perspectives 93 References 93 5 Graphene Field-Effect Transistors: Advanced Bioelectronic Devices for Sensing Applications 103
Kyung Ho Kim, Hyun Seok Song, Oh Seok Kwon, and Tai Hyun Park 5.1 Introduction 103 5.1.1 Bioelectronic Nose Using Olfactory Receptor-Conjugated Graphene 106 5.1.2 Bioelectronics for Diagnosis Using Bioprobe-Modified Graphene 112 5.1.3 Biosensors for Environmental Component Monitoring Using Graphene 116 5.2 Conclusion 120 Acknowledgments 120 References 120 6 Thin-Film Transistors Based on Reduced Graphene Oxide for Biosensing 125
Kai Bao, Ye Chen, Qiyuan He, and Hua Zhang 6.1 Introduction 125 6.2 Working Principle of TFT-Based Biosensing 126 6.3 TFTs Based on rGO for Biosensing 128 6.3.1 Protein Detection 128 6.3.2 Metal-Ion Detection 131 6.3.3 Nucleic Acid Detection 134 6.3.4 Small Biomolecular Biosensor 135 6.3.5 Living-Cell Biosensor 137 6.3.6 Gas Detection 138 6.4 Conclusion 140 References 142 7 Towards Graphene-FET Health Sensors: Hardware and Implementation Considerations 149
Nicholas V. Apollo and Hualin Zhan 7.1 Introduction to Health Sensing 149 7.2 Graphene-FET in Liquid for Sensing 151 7.2.1 Graphene Transistors 153 7.2.2 Graphene Hall Structures in Liquid 156 7.2.3 Graphene Membrane Transistors 159 7.3 Device Implementation Considerations 160 7.3.1 Hardware and Instrumentation 160 7.3.2 Biostability and Biocompatibility 162 7.3.3 Medical Imaging Compatibility 163 References 164 8 Quadratic Fit Analysis of the Nonlinear Transconductance of Disordered Bilayer Graphene Field-Effect Biosensors Functionalized with Pyrene Derivatives 169
Sung Oh Woo, Sakurako Tani, and Yongki Choi 8.1 Introduction 169 8.2 Fabrication of Graphene-Based Field-Effect Biosensors 170 8.3 Fundamental Sensing Parameters of Graphene-Based Field-Effect Biosensors 173 8.4 Disordered Bilayer Graphene Field-Effect Biosensors Functionalized with Pyrene Derivatives 174 8.5 Quadratic Fit Analysis of the Nonlinear Transconductance of Disordered Bilayer Graphene Field-Effect Biosensors 177 8.6 Conclusion 181 Acknowledgment 181 References 182 9 Theoretical and Experimental Characterization of Molecular Self-Assembly on Graphene Films 185
Kishan Thodkar, Pierre Cazade, and Damien Thompson 9.1 Introduction 185 9.2 Experimental Tools to Characterize Molecular Functionalization of Graphene 186 9.2.1 Considering the Three Distinct Techniques Available for Functionalizing Graphene Are the Outcomes of the Three Functionalization Techniques Consistent, Similar, Reproducible Across all Three Techniques? 187 9.2.2 What Tools and Methods Are Available to Perform Such a Characterization of Molecular Self-Assembly Across the Nano to Macro Scale? 188 9.3 Atomistic Insights to Guide Molecular Functionalization of Graphene 196 References 203 10 The Holy Grail of Surface Chemistry of C VD Graphene: Effect on Sensing of cTNI as Model Analyte 207
Adrien Hugo, Teresa Rodrigues, Marie-Helen Polte, Yann R. Leroux, Rabah Boukherroub, Wolfgang Knoll, and Sabine Szunerits 10.1 Introduction 207 10.2 General Overview of C VD Graphene Production, Substrate Transfer and Characterization 210 10.3 Evaluation of Graphene Topographical Quality 212 10.4 CVD Graphene for FET-Based Sensing 214 10.4.1 Diazonium Chemistry on CVD Graphene 217 10.4.2 Pyrene Chemistry on CVD Graphene 220 10.5 Conclusion 225 References 226 11 Sensing Mechanisms in Graphene Field-Effect Transistors Operating in Liquid 231
Tilmann J. Neubert and Kannan Balasubramanian 231 11.1 Introduction 231 11.2 Field-Effect Operation in Liquid Compared to Operation in Air 232 11.3 Caveats When Operating FETs in Liquid 234 11.4 Graphene FETs in Liquid 235 11.5 Measurement Modes 236 11.6 Using FETs for Sensing in Liquid – Sensing Mechanisms 238 11.7 The Electrochemical Perspective 241 11.8 The GLI and pH Sensing 245 11.9 Detection of Nucleic Acids 246 11.10 Other Examples 247 11.11 Concluding Remarks 248 References 248 12 Surface Modification Strategies to Increase the Sensing Length in Electrolyte-Gated Graphene Field-Effect Transistors 251
Juliana Scotto, Wolfgang Knoll, Waldemar A. Marmisollé, and Omar Azzaroni 12.1 Introduction 251 12.2 Ion-Exclusion and Donnan Potential 253 12.3 Surface Modification with Polymer Films 255 12.4 Surface Modification with Lipid Layers 258 12.5 Surface Modification with Mesoporous Materials 260 12.6 Kinetic Cost of Extending the Sensing Length 262 12.7 Conclusions 265 References 266 13 Hybridized Graphene Field-Effect Transistors for Gas Sensing Applications 271
Radha Bhardwaj and Arnab Hazra 271 13.1 Introduction 271 13.2 Graphene 272 13.3 Graphene FET 272 13.4 Graphene in Gas Sensing 274 13.5 Graphene FET for Gas Sensing 275 13.6 Hybrid Graphene FET for Gas Sensing 277 13.7 Conclusion 281 Acknowledgments 281 References 281 14 Polyelectrolyte-Enzyme Assemblies Integrated into Graphene Field-Effect Transistors for Biosensing Applications 285
Esteban Piccinini, Gonzalo E. Fenoy, Wolfgang Knoll, Waldemar A. Marmisollé, and Omar Azzaroni 14.1 Introduction 285 14.2 Field-Effect Transistors Based on Reduced Graphene Oxide 286 14.3 Enzyme-Based GFET Sensors Fabricated via Layer-by-Layer Assembly 287 14.3.1 Layer-by-Layer (LbL) Assemblies of Polyethylenimine and Urease onto Reduced Graphene-Oxide-Based Field-Effect Transistors (rGO FETs) for the Detection of Urea 288 14.3.2 Ultrasensitive Sensing Through Enzymatic Cascade Reactions on Graphene-Based FETs 292 14.4 Conclusions 296 References 297 15 Graphene Field-Effect Transistor Biosensor for Detection of Heart Failure-Related Biomarker in Whole Blood 301
Jiahao Li, Yongmin Lei, Zhi-Yong Zhang, and Guo-Jun Zhang 15.1 Introduction 301 15.2 Experimental Systems and Procedures 304 15.2.1 Fabrication of GFET Sensor 304 15.2.2 Decoration of Platinum Nanoparticles 304 15.2.3 Surface Functionalization 305 15.2.4 Immunodetection in Whole Blood 305 15.2.5 Electrical Measurements 305 15.3 Sensing Principle of GFET for BNP Detection 306 15.4 Device Characterization 306 15.5 Sensing Performance 308 15.5.1 Stability and Reproducibility 308 15.5.2 Selectivity 309 15.5.3 Sensitivity 309 15.6 Clinical Application Prospects 311 15.7 Advantages, Limitations, and Outlook of the FET-Based BNP Assay 311 References 313 16 Enzymatic Biosensors Based on the Electrochemical Functionalization of Graphene Field-Effect Transistors with Conducting Polymers 317
Gonzalo E. Fenoy, Esteban Piccinini, Wolfgang Knoll, Waldemar A. Marmisollé, and Omar Azzaroni 16.1 Introduction 317 16.2 Functionalization of Graphene Transistors with Poly(3-aminobenzylamine-co-aniline) Nanofilms 318 16.3 Construction of Acetylcholine Biosensors Based on GFET Devices Functionalized with Electropolymerized Poly(3-amino-benzylamineco-aniline) Nanofilms 322 16.4 Glucose Detection by Graphene Field-Effect Transistors Functionalized with Electropolymerized Poly(3-amino-benzylamine-co-aniline) Nanofilms 327 16.5 Conclusions 332 References 333 17 Graphene Field-Effect Transistors for Sensing Stress and Fatigue Biomarkers 339
Biddut K. Sarker, Cheri M. Hampton, and Lawrence F. Drummy 17.1 Introduction 339 17.2 Molecular Biomarkers 341 17.3 Graphene Field-Effect Transistor Based Biosensors 343 17.3.1 Graphene 343 17.3.2 Structure of Graphene Field-Effect Transistors 345 17.3.3 Sensing Mechanism of GFET Biosensors 346 17.4 GFET Biosensor Fabrication 348 17.4.1 Graphene Production 348 17.4.2 Device Fabrication 349 17.4.3 Graphene Functionalization 350 17.5 GFET-Based Stress and Fatigue Biosensors 353 17.6 Flexible, Wearable GFET Biosensors, and Biosensor Systems 358 17.7 Current Challenges and Future Perspective 362 17.7.1 Debye Length Screening 362 17.7.2 Device-to-Device Variability 366 17.7.3 Short Lifetime and Reusability Issue 366 17.8 Conclusion 367 References 367 18 Highly Sensitive Pathogen Detection by Graphene Field-Effect Transistor Biosensors Toward Point-of-Care-Testing 373
Shota Ushiba, Takao Ono, Yasushi Kanai, Naruto Miyakawa, Shinsuke Tani, Hiroshi Ueda, Masahiko Kimura, and Kazuhiko Matsumoto 18.1 Introduction 373 18.2 Toward Detection of Pathogens by Mimicking Cell Surfaces 374 18.2.1 Introduction 374 18.2.2 Fabrication of Sialoglycan-Functionalized GFETs 375 18.2.3 Evaluation of Sialoglycan-Functionalized GFETs 375 18.3 Signal Enhancement in GFETs 377 18.3.1 Sensitivity Enhancement by Increasing Receptor Density 377 18.3.1.1 Case of Linkers 377 18.3.1.2 Basis for Evaluation of Linker-Based Performance Enhancement 378 18.3.1.3 Evaluation of Performance Enhancement by Linkers 378 18.3.2 Ultrasensitive Detection of Small Antigens by Open-Sandwich Immunoassay on GFETs 380 18.3.2.1 Principle of Open-Sandwich (OS) Immunoassay 380 18.3.2.2 Advantages of OS-IAs with GFETs 380 18.3.2.3 Antibody Fragments and Device Fabrication 381 18.3.2.4 OS-IAs on GFETs 382 18.3.2.5 OS-IAs on GFETs in Human Serum 382 18.3.3 Real-Time Measurement of Enzyme Reaction in Microdroplets Using GFETs and Its Application to Pathogen Detection 384 18.3.3.1 Introduction 384 18.3.3.2 Measurement Mechanism and Model Measurement System 385 18.4 Practical Issues: Baseline Drift and Inspection Methods 387 18.4.1 Drift Suppression and Compensation of GFET Biosensors 388 18.4.1.1 Drift Suppression in GFETs by Cation Doping 388 18.4.1.2 Drift Compensation by State-Space Modeling 390 18.4.2 Deep-Learning-Based Optical Inspection of GFETs 393 18.5 Conclusion 398 References 398 19 High-Performance Detection of Extracellular Vesicles Using Graphene Field-Effect Transistor Biosensor 405
Ding Wu, Yi Yu, Zhi-Yong Zhang, and Guo-Jun Zhang 19.1 What is Extracellular Vesicles 405 19.2 The Clinical Significance of Extracellular Vesicles 406 19.3 Introduction to Graphene Field-Effect Transistor Biosensor 406 19.4 GFET Biosensor for High-Performance Detection of Extracellular Vesicles 407 19.4.1 Detection of the Overall Level of Microvesicles Using GFET Biosensor 408 19.4.2 Specific Detection of Hepatocellular Carcinoma-Derived Microvesicles Using Dual-Aptamer Modified GFET Biosensor 409 19.4.3 Label-Free Detection of Cancerous Exosomes Using GFET Biosensor 410 19.5 Some Prospects for Graphene Field-Effect Transistor Biosensor 411 References 412 Index 417

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