Toolbox of Advanced Atomic Layer Deposition Processes for Tailoring Large-Area MoS₂ Thin Films at 150 °C

Two-dimensional MoS₂ is a promising material for applications, including electronics and electrocatalysis. However, scalable methods capable of depositing MoS₂ at low temperatures are scarce. Herein, we present a toolbox of advanced plasma-enhanced atomic layer deposition (ALD) processes, producing wafer-scale polycrystalline MoS₂ films of accurately controlled thickness. Our ALD processes are based on two individually controlled plasma exposures, one optimized for deposition and the other for modification. In this way, film properties can be tailored toward different applications at a very low deposition temperature of 150 °C. For the modification step, either H₂ or Ar plasma can be used to combat excess sulfur incorporation and crystallize the films. Using H₂ plasma, a higher degree of crystallinity compared with other reported low-temperature processes is achieved. Applying H₂ plasma steps periodically instead of every ALD cycle allows for control of the morphology and enables deposition of smooth, polycrystalline MoS₂ films. Using an Ar plasma instead, more disordered MoS₂ films are deposited, which show promise for the electrochemical hydrogen evolution reaction. For electronics, our processes enable control of the carrier density from 6 × 10¹⁶ to 2 × 10²¹ cm^-3 with Hall mobilities up to 0.3 cm² V^-1 s^-1. The process toolbox forms a basis for rational design of low-temperature transition metal dichalcogenide deposition processes compatible with a range of substrates and applications.