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Title: In situ edge engineering in two-dimensional transition metal dichalcogenides

Exerting synthetic control over the edge structure and chemistry of two-dimensional (2D) materials is of critical importance to direct the magnetic, optical, electrical, and catalytic properties for specific applications. Here in this study, we directly image the edge evolution of pores in Mo 1-xW xSe 2 monolayers via atomic-resolution in situ scanning transmission electron microscopy (STEM) and demonstrate that these edges can be structurally transformed to theoretically predicted metastable atomic configurations by thermal and chemical driving forces. Density functional theory calculations and ab initio molecular dynamics simulations explain the observed thermally induced structural evolution and exceptional stability of the four most commonly observed edges based on changing chemical potential during thermal annealing. Finally, the coupling of modeling and in situ STEM imaging in changing chemical environments demonstrated here provides a pathway for the predictive and controlled atomic scale manipulation of matter for the directed synthesis of edge configurations in Mo 1-x W x Se 2 to achieve desired functionality.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ;  [2] ; ORCiD logo [1] ; ORCiD logo [1] ;  [3] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  2. Institute for Basic Science (IBS), Ulsan (Republic of Korea). Center for Multidimensional Carbon Materials (CMCM)
  3. Institute for Basic Science (IBS), Ulsan (Republic of Korea). Center for Multidimensional Carbon Materials (CMCM); Ulsan National Institute of Science and Technology (UNIST), Ulsan (Republic of Korea). School of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1474652

Sang, Xiahan, Li, Xufan, Zhao, Wen, Dong, Jichen, Rouleau, Christopher M., Geohegan, David B., Ding, Feng, Xiao, Kai, and Unocic, Raymond R.. In situ edge engineering in two-dimensional transition metal dichalcogenides. United States: N. p., Web. doi:10.1038/s41467-018-04435-x.
Sang, Xiahan, Li, Xufan, Zhao, Wen, Dong, Jichen, Rouleau, Christopher M., Geohegan, David B., Ding, Feng, Xiao, Kai, & Unocic, Raymond R.. In situ edge engineering in two-dimensional transition metal dichalcogenides. United States. doi:10.1038/s41467-018-04435-x.
Sang, Xiahan, Li, Xufan, Zhao, Wen, Dong, Jichen, Rouleau, Christopher M., Geohegan, David B., Ding, Feng, Xiao, Kai, and Unocic, Raymond R.. 2018. "In situ edge engineering in two-dimensional transition metal dichalcogenides". United States. doi:10.1038/s41467-018-04435-x. https://www.osti.gov/servlets/purl/1474652.
@article{osti_1474652,
title = {In situ edge engineering in two-dimensional transition metal dichalcogenides},
author = {Sang, Xiahan and Li, Xufan and Zhao, Wen and Dong, Jichen and Rouleau, Christopher M. and Geohegan, David B. and Ding, Feng and Xiao, Kai and Unocic, Raymond R.},
abstractNote = {Exerting synthetic control over the edge structure and chemistry of two-dimensional (2D) materials is of critical importance to direct the magnetic, optical, electrical, and catalytic properties for specific applications. Here in this study, we directly image the edge evolution of pores in Mo1-xW xSe2 monolayers via atomic-resolution in situ scanning transmission electron microscopy (STEM) and demonstrate that these edges can be structurally transformed to theoretically predicted metastable atomic configurations by thermal and chemical driving forces. Density functional theory calculations and ab initio molecular dynamics simulations explain the observed thermally induced structural evolution and exceptional stability of the four most commonly observed edges based on changing chemical potential during thermal annealing. Finally, the coupling of modeling and in situ STEM imaging in changing chemical environments demonstrated here provides a pathway for the predictive and controlled atomic scale manipulation of matter for the directed synthesis of edge configurations in Mo1-x W x Se2 to achieve desired functionality.},
doi = {10.1038/s41467-018-04435-x},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {5}
}

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996
  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Vapour phase growth and grain boundary structure of molybdenum disulphide atomic layers
journal, June 2013
  • Najmaei, Sina; Liu, Zheng; Zhou, Wu
  • Nature Materials, Vol. 12, Issue 8, p. 754-759
  • DOI: 10.1038/nmat3673

Projector augmented-wave method
journal, December 1994

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Anomalous Strength Characteristics of Tilt Grain Boundaries in Graphene
journal, November 2010

Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts
journal, July 2007
  • Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J.
  • Science, Vol. 317, Issue 5834, p. 100-102
  • DOI: 10.1126/science.1141483

Single-layer MoS2 transistors
journal, January 2011
  • Radisavljevic, B.; Radenovic, A.; Brivio, J.
  • Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
  • DOI: 10.1038/nnano.2010.279

Two-dimensional gas of massless Dirac fermions in graphene
journal, November 2005
  • Novoselov, K. S.; Geim, A. K.; Morozov, S. V.
  • Nature, Vol. 438, Issue 7065, p. 197-200
  • DOI: 10.1038/nature04233