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Title: Edge-Controlled Growth and Etching of Two-Dimensional GaSe Monolayers

Understanding the atomistic mechanisms governing the growth of two-dimensional (2D) materials is of great importance in guiding the synthesis of wafer-sized, single-crystalline, high-quality 2D crystals and heterostructures. Etching, in many cases regarded as the reverse process of material growth, has been used to study the growth kinetics of graphene. In this paper, we explore a growth–etching–regrowth process of monolayer GaSe crystals, including single-crystalline triangles and irregularly shaped domains formed by merged triangles. We show that the etching begins at a slow rate, creating triangular, truncated triangular, or hexagonally shaped holes that eventually evolve to exclusively triangles that are rotated 60° with respect to the crystalline orientation of the monolayer triangular crystals. The regrowth occurs much faster than etching, reversibly filling the etched holes and then enlarging the size of the monolayer crystals. A theoretical model developed based on kinetic Wulff construction (KWC) theory and density functional theory (DFT) calculations accurately describe the observed morphology evolution of the monolayer GaSe crystals and etched holes during the growth and etching processes, showing that they are governed by the probability of atom attachment/detachment to/from different types of edges with different formation energies of nucleus/dents mediated by chemical potential difference Δμ between Ga andmore » Se. Finally, our growth–etching–regrowth study provides not only guidance to understand the growth mechanisms of 2D binary crystals but also a potential method for the synthesis of large, shape-controllable, high-quality single-crystalline 2D crystals and their lateral heterostructures.« less
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  2. Inst. for Basic Science (IBS), Ulsan (Korea, Republic of). Center for Multidimensional Carbon Materials (CMCM)
  3. (UNIST), Ulsan (Korea, Republic of). School of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
AC05-00OR22725; IBS-R019-D1
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 1; Journal ID: ISSN 0002-7863
American Chemical Society (ACS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Inst. for Basic Science (IBS), Ulsan (Korea, Republic of)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Inst. for Basic Science (Korea, Republic of)
Contributing Orgs:
Ulsan National Inst. of Science and Technology (UNIST), Ulsan (Korea, Republic of)
Country of Publication:
United States
OSTI Identifier: