TY - JOUR
T1 - Reactivity of Sulfur Molecules on MoO3 (010) Surface
AU - Misawa, Masaaki
AU - Tiwari, Subodh
AU - Hong, Sungwook
AU - Krishnamoorthy, Aravind
AU - Shimojo, Fuyuki
AU - Kalia, Rajiv K.
AU - Nakano, Aiichiro
AU - Vashishta, Priya
N1 - Funding Information:
This work was supported as part of the Computational Materials Sciences Program funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award Number DE-SC00014607. The work in Kumamoto was supported by KAKENHI (16K05478) and grant-in-aid for JSPS research fellows (16J05234). The simulations were performed at the Center for High Performance Computing of the University of Southern California.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/12/21
Y1 - 2017/12/21
N2 - Two-dimensional and layered MoS2 is a promising candidate for next-generation electric devices due to its unique electronic, optical, and chemical properties. Chemical vapor deposition (CVD) is the most effective way to synthesize MoS2 monolayer on a target substrate. During CVD synthesis, sulfidation of MoO3 surface is a critical reaction step, which converts MoO3 to MoS2. However, initial reaction steps for the sulfidation of MoO3 remain to be fully understood. Here, we report first-principles quantum molecular dynamics (QMD) simulations for the initiation dynamics of sulfidation of MoO3 (010) surface using S2 and S8 molecules. We found that S2 molecule is much more reactive on the MoO3 surface than S8 molecule. Furthermore, our QMD simulations revealed that a surface O-vacancy on the MoO3 surface makes the sulfidation process preferable kinetically and thermodynamically. Our work clarifies an essential role of surface defects to initiate and accelerate the reaction of MoO3 and gas-phase sulfur precursors for CVD synthesis of MoS2 layers.
AB - Two-dimensional and layered MoS2 is a promising candidate for next-generation electric devices due to its unique electronic, optical, and chemical properties. Chemical vapor deposition (CVD) is the most effective way to synthesize MoS2 monolayer on a target substrate. During CVD synthesis, sulfidation of MoO3 surface is a critical reaction step, which converts MoO3 to MoS2. However, initial reaction steps for the sulfidation of MoO3 remain to be fully understood. Here, we report first-principles quantum molecular dynamics (QMD) simulations for the initiation dynamics of sulfidation of MoO3 (010) surface using S2 and S8 molecules. We found that S2 molecule is much more reactive on the MoO3 surface than S8 molecule. Furthermore, our QMD simulations revealed that a surface O-vacancy on the MoO3 surface makes the sulfidation process preferable kinetically and thermodynamically. Our work clarifies an essential role of surface defects to initiate and accelerate the reaction of MoO3 and gas-phase sulfur precursors for CVD synthesis of MoS2 layers.
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U2 - 10.1021/acs.jpclett.7b03011
DO - 10.1021/acs.jpclett.7b03011
M3 - Article
C2 - 29220193
AN - SCOPUS:85039037688
VL - 8
SP - 6206
EP - 6210
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 24
ER -