All-solution processing of large-area organic electronics requires multiple steps of patterning and stacking of various device components. Here, we report the fabrication of highly integrated arrays of polymer thin-film transistors and logic gates entirely through a series of solution processes. The fabrication is done using a three-dimensional crosslinker in tetrahedral geometry containing four photocrosslinkable azide moieties, referred to as 4Bx. 4Bx can be mixed with a variety of solution-processable electronic materials (polymer semiconductors, polymer insulators, and metal nanoparticles) and generate crosslinked network under exposure to UV. Fully crosslinked network film can be formed even at an unprecedentedly small loading, which enables preserving the inherent electrical and structural characteristics of host material. Because the crosslinked electronic component layers are strongly resistant to chemical solvents, micropatterning the layers at high resolution as well as stacking the layers on top of each other by series of solution processing steps is possible.

We report high-performance top-gate bottom-contact flexible polymer field-effect transistors (FETs) fabricated by flow-coating diketopyrrolopyrrole (DPP)-based and naphthalene diimide (NDI)-based polymers (P(DPP2DT-T2), P(DPP2DT-TT), P(DPP2DT-DTT), P(NDI2OD-T2), P(NDI2OD-F2T2), and P(NDI2OD-Se2)) as semiconducting channel materials. All of the polymers displayed good FET characteristics with on/off current ratios exceeding 10. The highest hole mobility of 1.51 cm V s and the highest electron mobility of 0.85 cm V s were obtained from the P(DPP2DT-T2) and P(NDI2OD-Se2) polymer FETs, respectively. The impacts of the polymer structures on the FET performance are well-explained by the interplay between the crystallinity, the tendency of the polymer backbone to adopt an edge-on orientation, and the interconnectivity of polymer fibrils in the film state. Additionally, we demonstrated that all of the flexible polymer-based FETs were highly resistant to tensile stress, with negligible changes in their carrier mobilities and on/off ratios after a bending test. Conclusively, these high-performance, flexible, and durable FETs demonstrate the potential of semiconducting conjugated polymers for use in flexible electronic applications.

Recently, combinations of 2D van der Waals (2D vdW) materials and organic materials have attracted attention because they facilitate the formation of various heterojunctions with excellent interface quality owing to the absence of dangling bonds on their surface. In this work, a double negative differential resistance (D-NDR) characteristic of a hybrid 2D vdW/organic tunneling device consisting of a hafnium disulfide/pentacene heterojunction and a 3D pentacene resistor is reported. This D-NDR phenomenon is achieved by precisely controlling an NDR peak voltage with the pentacene resistor and then integrating two distinct NDR devices in parallel. Then, the operation of a controllable-gain amplifier configured with the D-NDR device and an n-channel transistor is demonstrated using the Cadence Spectre simulation platform. The proposed D-NDR device technology based on a hybrid 2D vdW/organic heterostructure provides a scientific foundation for various circuit applications that require the NDR phenomenon.

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In this study, the poly (2,4,6,8-tetramethyl-2,4,6,8-tetravinylcyclotetrasiloxane-co-cyclohexyl methacrylate) [p(V4D4-co-CHMA)] copolymer was developed for use as a gate dielectric in molybdenum disulfide (MoS 2 ) field-effect transistors (FETs). The p(V4D4-co-CHMA) copolymer was synthesized via the initiated chemical vapor deposition (iCVD) of two types of monomers: 2,4,6,8-tetramethyl-2,4,6,8tetravinylcyclotetrasiloxane (V4D4) and cyclohexyl methacrylate (CHMA). Four vinyl groups of V4D4 monomers and cyclohexyl groups of CHMA monomers were introduced to enhance the electrical strength of gate dielectrics through the formation of a highly crosslinked network and to reduce the charge trap densities at the MoS 2 −dielectric interface, respectively. The iCVD-grown p(V4D4-co-CHMA) copolymer films yielded a dielectric constant of 2.3 and a leakage current of 3.8 × 10 −11 A/cm 2 at 1 MV/cm. The resulting MoS 2 FETs with p(V4D4-co-CHMA) gate dielectrics exhibited excellent electrical properties, including an electron mobility of 35.1 cm 2 /V s, a subthreshold swing of 0.2 V/dec, and an on−off current ratio of 2.6 × 10 6 . In addition, the environmental and operational stabilities of MoS 2 FETs with p(V4D4-co-CHMA) top-gate dielectrics were superior to those of devices with SiO 2 back-gate dielectrics. The use of iCVD-grown copolymer gate dielectrics as demonstrated in this study provides a novel approach to realizing next-generation two-dimensional electronics.