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Title: Growth Mechanisms of Anisotropic Layered Group IV Chalcogenides on van der Waals Substrates for Energy Conversion Applications

Abstract

Two-dimensional group IV monochalcogenide semiconductors (SnX, GeX; X = S, Se) are of fundamental interest due to their anisotropic crystal structure and predicted unique characteristics such as very large exciton binding energies and multiferroic order possibly up to above room temperature. Whereas growth on reactive supports produces mostly standing flakes, deposition on van der Waals (vdW) substrates can yield basal-plane oriented layered crystals. But so far, this approach invariably resulted in flakes that are several atomic layers thick, and the synthesis of monolayers has remained elusive. Here, we use in situ microscopy during molecular beam epitaxy of SnS on graphite and graphene to establish the origin of this predominant multilayer growth. The enhanced reactivity of group IV chalcogenide layers causes adsorption of precursor molecules primarily on the initial SnS nuclei instead of the vdW support. On graphite, this unusual imbalance in the material supply is the primary cause for fast vertical growth. Experiments on graphene/Ru(0001) suggest increased adsorption on the vdW substrate, which enables enhanced lateral SnS growth. As a result, the fundamental insight obtained here provides a basis for identifying conditions for the scalable synthesis of single-layer group IV monochalcogenides and guides the growth of high-quality multilayer films ofmore » interest for applications in energy conversion, optoelectronics, and thermoelectrics.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Nebraska-Lincoln, Lincoln, NE (United States). Dept. of Electrical and Computer Engineering
  2. Univ. of Nebraska-Lincoln, Lincoln, NE (United States). Dept. of Mechanical and Materials Engineering
Publication Date:
Research Org.:
Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1573816
Grant/Contract Number:  
[SC0016343]
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Nano Materials
Additional Journal Information:
[ Journal Volume: 1; Journal Issue: 6]; Journal ID: ISSN 2574-0970
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; semiconductor; 2D crystal; low-energy electron microscopy; adsorption; van der Waals growth; anisotropy

Citation Formats

Sutter, Peter, and Sutter, Eli. Growth Mechanisms of Anisotropic Layered Group IV Chalcogenides on van der Waals Substrates for Energy Conversion Applications. United States: N. p., 2018. Web. doi:10.1021/acsanm.8b00660.
Sutter, Peter, & Sutter, Eli. Growth Mechanisms of Anisotropic Layered Group IV Chalcogenides on van der Waals Substrates for Energy Conversion Applications. United States. doi:10.1021/acsanm.8b00660.
Sutter, Peter, and Sutter, Eli. Thu . "Growth Mechanisms of Anisotropic Layered Group IV Chalcogenides on van der Waals Substrates for Energy Conversion Applications". United States. doi:10.1021/acsanm.8b00660. https://www.osti.gov/servlets/purl/1573816.
@article{osti_1573816,
title = {Growth Mechanisms of Anisotropic Layered Group IV Chalcogenides on van der Waals Substrates for Energy Conversion Applications},
author = {Sutter, Peter and Sutter, Eli},
abstractNote = {Two-dimensional group IV monochalcogenide semiconductors (SnX, GeX; X = S, Se) are of fundamental interest due to their anisotropic crystal structure and predicted unique characteristics such as very large exciton binding energies and multiferroic order possibly up to above room temperature. Whereas growth on reactive supports produces mostly standing flakes, deposition on van der Waals (vdW) substrates can yield basal-plane oriented layered crystals. But so far, this approach invariably resulted in flakes that are several atomic layers thick, and the synthesis of monolayers has remained elusive. Here, we use in situ microscopy during molecular beam epitaxy of SnS on graphite and graphene to establish the origin of this predominant multilayer growth. The enhanced reactivity of group IV chalcogenide layers causes adsorption of precursor molecules primarily on the initial SnS nuclei instead of the vdW support. On graphite, this unusual imbalance in the material supply is the primary cause for fast vertical growth. Experiments on graphene/Ru(0001) suggest increased adsorption on the vdW substrate, which enables enhanced lateral SnS growth. As a result, the fundamental insight obtained here provides a basis for identifying conditions for the scalable synthesis of single-layer group IV monochalcogenides and guides the growth of high-quality multilayer films of interest for applications in energy conversion, optoelectronics, and thermoelectrics.},
doi = {10.1021/acsanm.8b00660},
journal = {ACS Applied Nano Materials},
number = [6],
volume = [1],
place = {United States},
year = {2018},
month = {5}
}

Journal Article:
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