In this work, we develop a field-effect transistor with a two-dimensional channel made of a single graphene layer to achieve label-free detection of DNA hybridization down to attomolar concentration, while being able to discriminate a single nucleotide polymorphism (SNP). The SNP-level target specificity is achieved by immobilization of probe DNA on the graphene surface through a pyrene-derivative heterobifunctional linker. Biorecognition events result in a positive gate voltage shift of the graphene charge neutrality point. The graphene transistor biosensor displays a sensitivity of 24 mV/dec with a detection limit of 25 aM: the lowest target DNA concentration for which the sensor can discriminate between a perfect-match target sequence and SNP-containing one.

Ten years have passed since the beginning of graphene research. In this period we have witnessed breakthroughs both in fundamental and applied research. However, the development of graphene devices for mass production has not yet reached the same level of progress. The architecture of graphene field-effect transistors (FET) has not significantly changed, and the integration of devices at the wafer scale has generally not been sought. Currently, whenever an electrolyte-gated FET (EGFET) is used, an external, cumbersome, out-of-plane gate electrode is required. Here, an alternative architecture for graphene EGFET is presented. In this architecture, source, drain, and gate are in the same plane, eliminating the need for an external gate electrode and the use of an additional reservoir to confine the electrolyte inside the transistor active zone. This planar structure with an integrated gate allows for wafer-scale fabrication of high-performance graphene EGFETs, with carrier mobility up to 1800 cm(2) V(-1) s(-1). As a proof-of principle, a chemical sensor was achieved. It is shown that the sensor can discriminate between saline solutions of different concentrations. The proposed architecture will facilitate the mass production of graphene sensors, materializing the potential of previous achievements in fundamental and applied graphene research.

This work is on developing clean-room processes for the fabrication of electrolyte-gate graphene field-effect transistors at the wafer scale for biosensing applications. Our fabrication process overcomes two main issues: removing surface residues after graphene patterning and the dielectric passivation of metallic contacts. A graphene residue-free transfer process is achieved by using a pre-transfer, sacrificial metallic mask that protects the entire wafer except the areas around the channel, source, and drain, onto which the graphene film is transferred and later patterned. After the dissolution of the mask, clean gate electrodes are obtained. The multilayer SiO2/SiNx dielectric passivation takes advantage of the excellent adhesion of SiO2 to graphene and the substrate materials and the superior impermeability of SiNx. It hinders native nucleation centers and breaks the propagation of defects through the layers, protecting from prolonged exposition to all common solvents found in biochemistry work, contrary to commonly used polymeric passivation. Since wet etch does not allow the required level of control over the lithographic process, a reactive ion etching process using a sacrificial metallic stopping layer is developed and used for patterning the passivation layer. The process achieves devices with high reproducibility at the wafer scale.

No abstract

Since the discovery of graphene, and due to its unique properties, we have witnessed a growing interest in the use of graphene-based devices for applications in the most diverse areas, namely in biosensing, particularly in the detection of genetic material. DNA can bind directly to graphene without the need of a linker and that makes this platform highly interesting for biosensor development.Here, electrochemical chips consisting of 6 independent gold microelectrode arrays as working electrode, and platinum reference and counter electrodes were fabricated at the wafer scale and, after graphene transfer and patterning, were used in the detection of DNA hybridization. Combining the sensitivity of electrochemical impedance spectroscopy and the selectivity of DNA beacons, we were able to detect DNA hybridization in a linear range between 5 pM and 5 nM, which is in the relevant clinical range for many diseases, with sensitivity to single nucleotide polymorphism.