Asymmetric Chemical Functionalization of Top-Contact Electrodes: Tuning the Charge Injection for High-Performance MoS₂ Field-Effect Transistors and Schottky Diodes.

Abstract

The fabrication of high-performance (opto-)electronic devices based on 2D channel materials requires the optimization of the charge injection at electrode-semiconductor interfaces. While chemical functionalization with chemisorbed self-assembled monolayers has been extensively exploited to adjust the work function of metallic electrodes in bottom-contact devices, such a strategy has not been demonstrated for the top-contact configuration, despite the latter being known to offer enhanced charge-injection characteristics. Here, a novel contact engineering method is developed to functionalize gold electrodes in top-contact field-effect transistors (FETs) via the transfer of chemically pre-modified electrodes. The source and drain Au electrodes of the molybdenum disulfide (MoS₂ ) FETs are functionalized with thiolated molecules possessing different dipole moments. While the modification of the electrodes with electron-donating molecules yields a marked improvement of device performance, the asymmetric functionalization of the source and drain electrodes with different molecules with opposed dipole moment enables the fabrication of a high-performance Schottky diode with a rectification ratio of ≈10³ . This unprecedented strategy to tune the charge injection in top-contact MoS₂ FETs is of general applicability for the fabrication of high-performance (opto-)electronic devices, in which asymmetric charge injection is required, enabling tailoring of the device characteristics on demand.