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Title: Revealing the preferred interlayer orientations and stackings of two-dimensional bilayer gallium selenide crystals

Characterizing and controlling the interlayer orientations and stacking order of bilayer two-dimensional (2D) crystals and van der Waals (vdW) heterostructure is crucial to optimize their electrical and optoelectronic properties. The four polymorphs of layered gallium selenide (GaSe) that result from different layer stacking provide an ideal platform to study the stacking configurations in bilayer 2D crystals. Here, through a controllable vapor-phase deposition method we selectively grow bilayer GaSe crystals and investigate their two preferred 0° or 60° interlayer rotations. The commensurate stacking configurations (AA' and AB-stacking) in as-grown 2D bilayer GaSe crystals are clearly observed at the atomic scale and the Ga-terminated edge structure are identified for the first time by using atomic-resolution scanning transmission electron microscopy (STEM). Theoretical analysis of the interlayer coupling energetics vs. interlayer rotation angle reveals that the experimentally-observed orientations are energetically preferred among the bilayer GaSe crystal polytypes. Here, the combined experimental and theoretical characterization of the GaSe bilayers afforded by these growth studies provide a pathway to reveal the atomistic relationships in interlayer orientations responsible for the electronic and optical properties of bilayer 2D crystals and vdW heterostructures.
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Escuela Politecnica Nacional, Quito (Ecuador)
Publication Date:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 54; Journal Issue: 9; Journal ID: ISSN 1433-7851
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC)
Country of Publication:
United States
36 MATERIALS SCIENCE; gallium selenide; monolayer; interlayer orientation; stacking; vapour-phase deposition
OSTI Identifier: