The electrodeposition of MoS₂ from dichloromethane (CH₂Cl₂) using tetrabutylammonium tetrathiomolybdate ([NⁿBu₄]₂[MoS₄]) as a single source precursor is presented. The electrodeposition of MoS₂ from CH₂Cl₂ requires addition of a proton donor to the electrolyte and trimethylammonium chloride (Me₃NHCl) was used for this purpose. Electrochemical Quartz Crystal Microbalance (EQCM) experiments have been employed for a detailed study of the electrochemical mechanism and to study the role of the proton donor. EQCM reveals cathodic electrodeposition of MoS₂ and anodic deposition of MoS₃ as well as an additional corrosion process where the deposited MoS₃ strips back into solution. The electrodeposited MoS₂ films are amorphous in nature. All the films were found to be homogeneous in composition across the electrode area and to be reproducible between experiments. Annealing of the as-deposited films under a sulfur atmosphere results in crystalline MoS₂ as confirmed by energy dispersive X-ray spectroscopy (EDX), Raman spectroscopy and X-ray diffraction. The deposited films were smooth and planar, as observed with scanning electron microscopy (SEM), indicating a layer-by-layer growth typical of transition metal dichalogenides.

Developing novel techniques for depositing transition metal dichalcogenides is crucial for the industrial adoption of 2D materials in optoelectronics. In this work, the lateral growth of molybdenum disulfide (MoS₂) over an insulating surface is demonstrated using electrochemical deposition. By fabricating a new type of microelectrodes, MoS₂ 2D films grown from TiN electrodes across opposite sides are connected over an insulating substrate, hence, forming a lateral device structure through only one lithography and deposition step. Using a variety of characterization techniques, the growth rate of MoS₂ is shown to be highly anisotropic with lateral to vertical growth ratios exceeding 20‐fold. Electronic and photo‐response measurements on the device structures demonstrate that the electrodeposited MoS₂ layers behave like semiconductors, confirming their potential for photodetection applications. This lateral growth technique paves the way toward room temperature, scalable, and site‐selective production of various transition metal dichalcogenides and their lateral heterostructures for 2D materials‐based fabricated devices.