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Title: Atomic-Scale Insights into the Lateral and Vertical Epitaxial Growth in Two-Dimensional Pd2Se3–MoS2 Heterostructures

Abstract

Two-dimensional (2D) materials form heterostructures in both the lateral and vertical directions when two different materials are interfaced, but with totally different bonding mechanisms of covalent in-plane to van der Waal’s layered interactions. Understanding how the competition between lateral and vertical forces influences the epitaxial growth is important for future materials development of complex mixed layered heterostructures. In this study, we use atomic-resolution annular dark-field scanning transmission electron microscopy to study the detailed atomic arrangements at mixed 2D heterostructure interfaces composed of two semiconductors with distinctly different crystal symmetry and elemental composition, Pd2Se3:MoS2, in order to understand the role of different chemical bonds on the resultant epitaxy. Pd2Se3 is grown off the step edge in bilayer MoS2, and the vertical and lateral epitaxial relationships of the Pd2Se3–MoS2 heterostructures are investigated. We find that the similarity of geometry at the interface with one metal (Pd or Mo) atoms bonded with two chalcogens (S or Se) are the crucial factors to make the atomically stitched lateral junction of 2D heterostructures. In addition, the vertical van der Waal interactions that are normally dominant in layered materials can be overcome by in-plane forces if the interfacial atomic stitching is high in quality and lowmore » in defect density. This knowledge should help guide the approaches for improving the epitaxy in mixed 2D heterostructures and seamless stitching of in-plane 2D heterostructures with various complex monolayer structures.« less

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [3];  [1]; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Univ. of Oxford (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1881142
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 16; Journal Issue: 7; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; two-dimensional materials; defects; atomic structure; bonding; epitaxy; heterostructures; interfaces; lattices; palladium

Citation Formats

Park, Hyoju, Jung, Gang Seob, Ibrahim, Khaled M., Lu, Yang, Tai, Kuo-Lun, Coupin, Matthew, and Warner, Jamie H. Atomic-Scale Insights into the Lateral and Vertical Epitaxial Growth in Two-Dimensional Pd2Se3–MoS2 Heterostructures. United States: N. p., 2022. Web. doi:10.1021/acsnano.1c09019.
Park, Hyoju, Jung, Gang Seob, Ibrahim, Khaled M., Lu, Yang, Tai, Kuo-Lun, Coupin, Matthew, & Warner, Jamie H. Atomic-Scale Insights into the Lateral and Vertical Epitaxial Growth in Two-Dimensional Pd2Se3–MoS2 Heterostructures. United States. https://doi.org/10.1021/acsnano.1c09019
Park, Hyoju, Jung, Gang Seob, Ibrahim, Khaled M., Lu, Yang, Tai, Kuo-Lun, Coupin, Matthew, and Warner, Jamie H. Wed . "Atomic-Scale Insights into the Lateral and Vertical Epitaxial Growth in Two-Dimensional Pd2Se3–MoS2 Heterostructures". United States. https://doi.org/10.1021/acsnano.1c09019. https://www.osti.gov/servlets/purl/1881142.
@article{osti_1881142,
title = {Atomic-Scale Insights into the Lateral and Vertical Epitaxial Growth in Two-Dimensional Pd2Se3–MoS2 Heterostructures},
author = {Park, Hyoju and Jung, Gang Seob and Ibrahim, Khaled M. and Lu, Yang and Tai, Kuo-Lun and Coupin, Matthew and Warner, Jamie H.},
abstractNote = {Two-dimensional (2D) materials form heterostructures in both the lateral and vertical directions when two different materials are interfaced, but with totally different bonding mechanisms of covalent in-plane to van der Waal’s layered interactions. Understanding how the competition between lateral and vertical forces influences the epitaxial growth is important for future materials development of complex mixed layered heterostructures. In this study, we use atomic-resolution annular dark-field scanning transmission electron microscopy to study the detailed atomic arrangements at mixed 2D heterostructure interfaces composed of two semiconductors with distinctly different crystal symmetry and elemental composition, Pd2Se3:MoS2, in order to understand the role of different chemical bonds on the resultant epitaxy. Pd2Se3 is grown off the step edge in bilayer MoS2, and the vertical and lateral epitaxial relationships of the Pd2Se3–MoS2 heterostructures are investigated. We find that the similarity of geometry at the interface with one metal (Pd or Mo) atoms bonded with two chalcogens (S or Se) are the crucial factors to make the atomically stitched lateral junction of 2D heterostructures. In addition, the vertical van der Waal interactions that are normally dominant in layered materials can be overcome by in-plane forces if the interfacial atomic stitching is high in quality and low in defect density. This knowledge should help guide the approaches for improving the epitaxy in mixed 2D heterostructures and seamless stitching of in-plane 2D heterostructures with various complex monolayer structures.},
doi = {10.1021/acsnano.1c09019},
journal = {ACS Nano},
number = 7,
volume = 16,
place = {United States},
year = {Wed Jul 13 00:00:00 EDT 2022},
month = {Wed Jul 13 00:00:00 EDT 2022}
}

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