The noncovalent functionalization of two-dimensional materials (2DMs) with bespoke organic molecules is of central importance for future nanoscale electronic devices. Of particular interest is the incorporation of molecular functionalities that can modulate the physicochemical properties of the 2DMs via noninvasive external stimuli. In this study, we present the reversible modulation of the photoluminescence, spectroscopic properties (Raman), and charge transport characteristics of molybdenum disulfide (MoS2)-based devices via photoisomerization of a self-assembled monolayer of azobenzene-modified triazatriangulene molecules. The observed (opto)­electronic modulations are explained by the n-type doping of the MoS2 lattice induced by the photoisomerization of the highly ordered azobenzene monolayer. This novel behavior could have profound effects on future composite 2DM-based (opto)­electronics.

We present a novel maskless device fabrication technique for rapid prototyping of two-dimensional (2D)-based electronic materials. The technique is based on a thermally activated and self-developed cyclic polyphthalaldehyde (c-PPA) resist using a commercial Raman system and 532 nm laser illumination. Following the successful customization of electrodes to form field effect transistors based on MoS2 monolayers, the laser-induced electronic doping of areas beneath the metal contacts that were exposed during lithography was investigated using both surface potential mapping and device characterization. An effective change in the doping level was introduced depending on the laser intensity, i.e., low laser powers resulted in p-doping, while high laser powers resulted in n-doping. Fabricated devices present a low contact resistance down to 10 kΩ·μm at a back-gate voltage of V G = 80 V, which is attributed to the laser-induced n-type doping at the metal contact regions.