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Atomically layered transition metal dichalcogenides (TMDCs) exhibit a significant potential to enable next-generation low-cost transistor biosensors that permit single-molecule-level quantification of biomolecules. To realize such potential biosensing capability, device-oriented research is needed for calibrating the sensor responses to enable the quantification of the affinities/kinetics of biomolecule interactions. In this work, we demonstrated MoS2-based transistor biosensors capable of detecting tumor necrosis factor--alpha (TNF-α) with a detection limit as low as 60 fM. Such a detection limit was achieved in both linear and subthreshold regimes of MoS2 transistors. In both regimes, all sets of transistors exhibited consistent calibrated responses with respect to TNF-α concentration, and they resulted in a standard curve, from which the equilibrium constant of the antibody-(TNF-α) pair was extracted to be KD = 369 ± 48 fM. Based on this calibrated sensor model, the time-dependent binding kinetics was also measured and the association/dissociation rates of the antibody-(TNF-α) pair were extracted to be (5.03 ± 0.16) × 10(8) M(-1) s(-1) and (1.97 ± 0.08) × 10(-4) s(-1), respectively. This work advanced the critical device physics for leveraging the excellent electronic/structural properties of TMDCs in biosensing applications as well as the research capability in analyzing the biomolecule interactions with fM-level sensitivities.

Large-area few-layer-MoS2 device arrays are desirable for scale-up applications in nanoelectronics. Here we present a novel approach for producing orderly arranged, pristine few-layer MoS2 flakes, which holds significant potential to be developed into a nanomanufacturing technology that can be scaled up. We pattern bulk MoS2 stamps using lithographic techniques and subsequently transfer-print prepatterned MoS2 features onto pristine and plasma-charged SiO2 substrates. Our work successfully demonstrates the transfer printing of MoS2 flakes into ordered arrays over cm(2)-scale areas. Especially, the MoS2 patterns printed on plasma-charged substrates feature a regular edge profile and a narrow distribution of MoS2 flake thicknesses (i.e., 3.0 ± 1.9 nm) over cm(2)-scale areas. Furthermore, we experimentally show that our plasma-assisted printing process can be generally used for producing other emerging atomically layered nanostructures (e.g., graphene nanoribbons). We also demonstrate working n-type transistors made from printed MoS2 flakes that exhibit excellent properties (e.g., ON/OFF current ratio 10(5)-10(7), field-effect mobility on SiO2 gate dielectrics 6 to 44 cm(2)/(V s)) as well as good uniformity of such transistor parameters over a large area. Finally, with additional plasma treatment processes, we also show the feasibility of creation of p-type transistors as well as pn junctions in MoS2 flakes. This work lays an important foundation for future scale-up nanoelectronic applications of few-layer-MoS2 micro- and nanostructures.