Date of Award
Doctor of Philosophy (PhD)
Physics & Astronomy
Alan T. Johnson
Two dimensional materials have properties that make them ideal for applications in chemical and biomolecular sensing. Their high surface/volume ratio implies that all atoms are exposed to the environment, in contrast to three dimensional materials with most atoms shielded from interactions inside the bulk. Graphene additionally has an extremely high carrier mobility, even at ambient temperature and pressure, which makes it ideal as a transduction device. The work presented in this thesis describes large-scale fabrication of Graphene Field Effect Transistors (GFETs), their physical and chemical characterization, and their application as biomolecular sensors. Initially, work was focused on developing an easily scalable fabrication process. A large-area graphene growth, transfer and photolithography process was developed that allowed the scaling of production of devices from a few devices per single transfer in a chip, to over a thousand devices per transfer in a full wafer of fabrication. Two approaches to biomolecules sensing were then investigated, through nanoparticles and through chemical linkers.
Gold and platinum Nanoparticles were used as intermediary agents to immobilize a biomolecule. First, gold nanoparticles were monodispersed and functionalized with thiolated probe DNA to yield DNA biosensors with a detection limit of 1 nM and high specificity against noncomplementary DNA. Second, devices are modified with platinum nanoparticles and functionalized with thiolated genetically engineered scFv HER3 antibodies to realize a HER3 biosensor. Sensors retain the high affinity from the scFv fragment and show a detection limit of 300 pM.
We then show covalent and non-covalent chemical linkers between graphene and antibodies. The chemical linker 1-pyrenebutanoic acid succinimidyl ester (pyrene) stacks to the graphene by Van der Waals interaction, being a completely non-covalent interaction. The linker 4-Azide-2,3,5,6-tetrafluorobenzoic acid, succinimidyl ester (azide) is a photoactivated perfluorophenyl azide that covalently binds to graphene. A comparison is shown for genetically engineered scFv HER3 antibodies and show a low detection limit of 10 nM and 100 pM for the pyrene and azide, respectively. Finally, we use the azide linker to demonstrate a large-scale fabrication of a multiplexed array for Lyme disease. Simultaneous detection of a mixture of two target proteins of the Lyme disease bacterium (Borrelia burgdorferi), this is done by separating the antibodies corresponding to each target in the mixture to different regions of the chip. We show we can differentiate concentrations of the two targets.
Ducos, Pedro Jose, "Nano/biosensors Based On Large-Area Graphene" (2017). Publicly Accessible Penn Dissertations. 2263.