Chemical Vapor Deposition Synthesis of MoS2 Layers from the Direct Sulfidation of MoO3 Surfaces Using Reactive Molecular Dynamics Simulations

Sungwook Hong, Chunyang Sheng, Aravind Krishnamoorthy, Pankaj Rajak, Subodh Tiwari, Ken Ichi Nomura, Masaaki Misawa, Fuyuki Shimojo, Rajiv K. Kalia, Aiichiro Nakano, Priya Vashishta

Research output: Contribution to journalArticlepeer-review

38 Citations (Scopus)


Atomically thin MoS2 layer, a promising transition metal dichalcogenide (TMDC) material, has great potential for application in next-generation electronic and optoelectronic devices. Chemical vapor deposition (CVD) is the most effective technique for the synthesis of high-quality MoS2 layers. During CVD synthesis, monolayered MoS2 is generally synthesized by sulfidation of MoO3. Although qualitative reaction mechanisms for the sulfidation of MoO3 have been investigated by previous studies, the detailed reaction processes, including atomic-scale reaction pathways and growth kinetics, have yet to be fully understood. Here, we present quantum-mechanically informed and validated reactive molecular dynamics simulations of the direct sulfidation of MoO3 surfaces using S2 gas precursors. Our work clarifies the reaction mechanisms and kinetics of the sulfidation of MoO3 surfaces as follows: the reduction and sulfidation of MoO3 surfaces occur primarily at O-termination sites, followed by unsaturated Mo sites; these local reaction processes lead to nonuniform MoOxSy surface structures during the CVD process. After annealing the MoOxSy samples, the crystallized surface structures contain voids, and three different types of local surface complexes (MoOx, MoOxSy, and MoS2-like surface regions), depending on the fraction of S ingredients on the MoOxSy surface. These results, which have been validated by our reactive quantum molecular dynamics simulations and previous experimental results, provide valuable chemical insights into the CVD synthesis of large-scale and defect-free MoS2 layers and other layered TMDC materials.

Original languageEnglish
Pages (from-to)7494-7503
Number of pages10
JournalJournal of Physical Chemistry C
Issue number13
Publication statusPublished - Apr 5 2018
Externally publishedYes

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films


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