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The ability to modulate optical and electrical properties of two-dimensional (2D) semiconductors has sparked considerable interest in transition metal dichalcogenides (TMDs). Herein, we introduce a facile strategy for modulating optoelectronic properties of monolayer MoSe₂with external light. Photochromic diarylethene (DAE) molecules formed a 2-nm-thick uniform layer on MoSe₂, switching between its closed- and open-form isomers under UV and visible irradiation, respectively. We have discovered that the closed DAE conformation under UV has its lowest unoccupied molecular orbital energy level lower than the conduction band minimum of MoSe₂, which facilitates photoinduced charge separation at the hybrid interface and quenches photoluminescence (PL) from monolayer flakes. In contrast, open isomers under visible light prevent photoexcited electron transfer from MoSe₂to DAE, thus retaining PL emission properties. Alternating UV and visible light repeatedly show a dynamic modulation of optoelectronic signatures of MoSe₂. Conductive atomic force microscopy and Kelvin probe force microscopy also reveal an increase in conductivity and work function of MoSe₂/DAE with photoswitched closed-form DAE. These results may open new opportunities for designing new phototransistors and other 2D optoelectronic devices.

Transition metal dichalcogenides (TMDCs) have received much attention for optoelectronic applications because of their band gap transition from indirect to direct as they decrease from multilayer to monolayer. Recent studies have experimented with the use of photochromic molecules to optically control the charge transport of two-dimensional (2D) TMDCs. In this work, a numerical study using density functional theory has been performed to test the possibility to control the optical property of 2D TMDC monolayers with various photochromic molecules. When the photochromic molecule’s highest occupied molecular orbital (HOMO) or lowest unoccupied molecular orbital (LUMO) energy levels are within the band gap of 2D TMDC monolayers, holes or electrons will transport to the photochromic molecules, resulting in the reduction of excitons in the 2D TMDC monolayers. The reduced optical response can be recovered by going through reverse isomerization of the photochromic molecules. Molybdenum disulfide (MoS2) and tungsten diselenide (WSe2) monolayers were tested with various photochromic molecules including azobenzene, spiropyran, and diarylethenes (DAE 2 ethyl, DAE 5 ethyl, DAE 5 methyl). The systematic study presented in this work displays that MoS2-Spiropyran and every diarylethene derivative used in this study except MoS2-DAE 5 methyl exhibited photo-switchable behavior.

One of the most attractive features of 2D WSe₂is a tunability in its electronic and optoelectronic properties depending on the layer number. To harness such unique characteristics for device applications, high quality and easily processable heterojunctions are required and relevant layer‐number‐dependent properties must be understood. Herein, a study is reported on hybrid heterojunctions between 2D WSe₂and organic molecules from one‐step solution chemistry and their layer‐number‐dependent properties. Eosin Y (EY) dye is selected as a p‐dopant and uniformly stacked on mechanically exfoliated WSe₂flakes via van der Waals interaction, forming a hybrid heterojunction with a type II alignment. The EY‐WSe₂heterojunction shows significantly enhanced currents compared to pristine WSe₂with a lower barrier height and a longer effective screening length. The work function of the heterostructure is also lower than that of pristine WSe₂. The efficient exciton dissociation and doping effect by EY are confirmed by photocurrent and photoluminescence measurements, where WSe₂emission is markedly quenched by EY and exciton contribution decreases with layer number. These findings shed critical insights into layer‐number‐dependent electronic and optoelectronic properties of organic‐WSe₂layers and also provide simple yet effective means to construct transition metal dichalcogenide‐based heterostructures, which should be valuable for developing layered 2D devices.