Covalently interconnected transition metal dichalcogenide networks via defect engineering for high-performance electronic devices.

Abstract

Solution-processed semiconducting transition metal dichalcogenides are at the centre of an ever-increasing research effort in printed (opto)electronics. However, device performance is limited by structural defects resulting from the exfoliation process and poor inter-flake electronic connectivity. Here, we report a new molecular strategy to boost the electrical performance of transition metal dichalcogenide-based devices via the use of dithiolated conjugated molecules, to simultaneously heal sulfur vacancies in solution-processed transition metal disulfides and covalently bridge adjacent flakes, thereby promoting percolation pathways for the charge transport. We achieve a reproducible increase by one order of magnitude in field-effect mobility (µFE), current ratio (ION/IOFF) and switching time (τS) for liquid-gated transistors, reaching 10-2 cm2 V-1 s-1, 104 and 18 ms, respectively. Our functionalization strategy is a universal route to simultaneously enhance the electronic connectivity in transition metal disulfide networks and tailor on demand their physicochemical properties according to the envisioned applications.European Commission through the Graphene Flagship, the ERC Grants SUPRA2DMAT (GA-833707), FUTURE-PRINT (GA-694101), Hetero2D, GSYNCOR, the EU Grant Neurofibres, the Agence Nationale de la Recherche through the Labex projects CSC (ANR-10-LABX-0026 CSC) and NIE (ANR-11-LABX-0058 NIE) within the Investissement d’Avenir program (ANR-10-120 IDEX-0002-02), the International Center for Frontier Research in Chemistry (icFRC), EPSRC Grants EP/K01711X/1, EP/K017144/1, EP/N010345/1, EP/L016057/1, and the Faraday Institution. The HAADF-STEM characterization was carried out in the Advanced Microscopy Laboratory (Dublin), a Science Foundation Ireland (SFI) supported centre