Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling

Liu, Da-Jiang; Evans, James W.; Spurgeon, Peter M.; Thiel, Patricia A.

doi:10.1063/5.0006131

Title: Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling

Abstract

Ordering of different chalcogens, S, Se, and Te, on Au(111) exhibit broad similarities but also some distinct features, which must reflect subtle differences in relative values of the long-range pair and many-body lateral interactions between adatoms. We develop lattice-gas (LG) models within a cluster expansion framework, which includes about 50 interaction parameters. These LG models are developed based on density functional theory (DFT) analysis of the energetics of key adlayer configurations in combination with the Monte Carlo (MC) simulation of the LG models to identify statistically relevant adlayer motifs, i.e., model development is based entirely on theoretical considerations. The MC simulation guides additional DFT analysis and iterative model refinement. Given their complexity, development of optimal models is also aided by strategies from supervised machine learning. The model for S successfully captures ordering motifs over a broader range of coverage than achieved by previous models, and models for Se and Te capture the features of ordering, which are distinct from those for S. More specifically, the modeling for all three chalcogens successfully explains the linear adatom rows (also subtle differences between them) observed at low coverages of ~0.1 monolayer. The model for S also leads to a new possible explanation formore »« less

Authors:

^[1];

^[2]; Spurgeon, Peter M. ^[2];

^[2]

Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Publication Date:: Tue Jun 09 00:00:00 EDT 2020

Research Org.:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)

OSTI Identifier:: 1632685

Alternate Identifier(s):: OSTI ID: 1632722

Report Number(s):: IS-J-10,238
Journal ID: ISSN 0021-9606; TRN: US2201374

Grant/Contract Number:: AC02-07CH11358; AC02-05CH11231; CHE-1507223

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 152; Journal Issue: 22; Journal ID: ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Liu, Da-Jiang, Evans, James W., Spurgeon, Peter M., and Thiel, Patricia A. Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling.  United States: N. p., 2020. 
Web.  doi:10.1063/5.0006131.

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                    Liu, Da-Jiang, Evans, James W., Spurgeon, Peter M., & Thiel, Patricia A. Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling.  United States.  https://doi.org/10.1063/5.0006131

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                    Liu, Da-Jiang, Evans, James W., Spurgeon, Peter M., and Thiel, Patricia A. Tue .  
"Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling".  United States.  https://doi.org/10.1063/5.0006131.  https://www.osti.gov/servlets/purl/1632685.

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@article{osti_1632685,

  title        = {Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling},

  author       = {Liu, Da-Jiang and Evans, James W. and Spurgeon, Peter M. and Thiel, Patricia A.},

  abstractNote = {Ordering of different chalcogens, S, Se, and Te, on Au(111) exhibit broad similarities but also some distinct features, which must reflect subtle differences in relative values of the long-range pair and many-body lateral interactions between adatoms. We develop lattice-gas (LG) models within a cluster expansion framework, which includes about 50 interaction parameters. These LG models are developed based on density functional theory (DFT) analysis of the energetics of key adlayer configurations in combination with the Monte Carlo (MC) simulation of the LG models to identify statistically relevant adlayer motifs, i.e., model development is based entirely on theoretical considerations. The MC simulation guides additional DFT analysis and iterative model refinement. Given their complexity, development of optimal models is also aided by strategies from supervised machine learning. The model for S successfully captures ordering motifs over a broader range of coverage than achieved by previous models, and models for Se and Te capture the features of ordering, which are distinct from those for S. More specifically, the modeling for all three chalcogens successfully explains the linear adatom rows (also subtle differences between them) observed at low coverages of ~0.1 monolayer. The model for S also leads to a new possible explanation for the experimentally observed phase with a (5 × 5)-type low energy electron diffraction (LEED) pattern at 0.28 ML and to predictions for LEED patterns that would be observed with Se and Te at this coverage.},

  doi          = {10.1063/5.0006131},

  journal      = {Journal of Chemical Physics},

  number       = 22,

  volume       = 152,

  place        = {United States},

  year         = {Tue Jun 09 00:00:00 EDT 2020},

  month        = {Tue Jun 09 00:00:00 EDT 2020}

}

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Title: Structure of chalcogen overlayers on Au(111): Density functional theory and lattice-gas modeling

Abstract

Citation Formats

Adsorption of Te atoms on Au(1 1 1) and the emergence of an adatom-induced bound state journal, February 2017

The Structure of Atomic Sulfur Phases on Au(111) journal, June 2007

Density functional analysis of key energetics in metal homoepitaxy: Quantum size effects in periodic slab calculations journal, January 2010

Long-Range Periodicity of S/Au(111) Structures at Low and Intermediate Coverages journal, December 2013

Molecular alligator clips: a theoretical study of adsorption of S, Se and S–H on Au(111) journal, June 2003

Self-organization of S adatoms on Au(111): √3R30° rows at low coverage journal, July 2015

Indirect long-range oscillatory interaction between adsorbed atoms journal, July 1978

Long-ranged adsorbate-adsorbate interactions mediated by a surface-state band journal, December 1999

Linear Model Selection by Cross-validation journal, June 1993

Superstructures of Se adsorbates on Au(111): Scanning tunneling microscopy and spectroscopy study journal, July 2019

Formation of Two-Dimensional Copper Selenide on Cu(111) at Very Low Selenium Coverage journal, May 2016

Identification of an AgS2 Complex on Ag(110) journal, December 2019

Comparison of S-adsorption on (111) and (100) facets of Cu nanoclusters journal, October 2016

Self-Assembled Selenium Monolayers: From Nanotechnology to Materials Science and Adaptive Catalysis journal, November 2013

Investigations on Silver Sulfide journal, October 1953

Revisiting the S−Au(111) Interaction: Static or Dynamic? journal, March 2005

Oxygen and sulfur adsorption on vicinal surfaces of copper and silver: Preferred adsorption sites journal, March 2018

Comment on “oscillatory indirect interaction between adsorbed atoms — Non-asymptotic behavior in tight-binding models at realistic parameters” by K.H. Lau and W. Kohn journal, July 1978

Surface-state–mediated three-adsorbate interaction journal, July 2002

Long-Range Displacive Reconstruction of Au(110) Triggered by Low Coverage of Sulfur journal, August 2015

Formulation of Multicomponent Lattice Gas Model Cluster Expansions Parameterized on Ab Initio Data: An Introduction to the Ab Initio Mean-Field Augmented Lattice Gas Modeling Code journal, December 2019

Au(111) surface structures induced by adsorption: LEED I(E) analysis of (1×1) and (5×5) Au(111)–S phases journal, April 2013

Coverage Effects and the Nature of the Metal−Sulfur Bond in S/Au(111): High-Resolution Photoemission and Density-Functional Studies journal, January 2003

Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] journal, February 1997

Zur Thermodynamik von Schwefeldampf journal, August 1967

Reaction of Au(111) with Sulfur and Oxygen: Scanning Tunneling Microscopic Study journal, August 2005

Stabilization of X–Au–X Complexes on the Au(111) Surface: A Theoretical Investigation and Comparison of X = S, Cl, CH 3 S, and SiH 3 S journal, February 2017

Structural Investigation of the Interaction of Molecular Sulfur with Ag(111) journal, January 2007

Adsorption of Te atoms on Au(1 1 1) and the emergence of an adatom-induced bound state
journal, February 2017

The Structure of Atomic Sulfur Phases on Au(111)
journal, June 2007

Density functional analysis of key energetics in metal homoepitaxy: Quantum size effects in periodic slab calculations
journal, January 2010

Long-Range Periodicity of S/Au(111) Structures at Low and Intermediate Coverages
journal, December 2013

Molecular alligator clips: a theoretical study of adsorption of S, Se and S–H on Au(111)
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Self-organization of S adatoms on Au(111): √3R30° rows at low coverage
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Indirect long-range oscillatory interaction between adsorbed atoms
journal, July 1978

Long-ranged adsorbate-adsorbate interactions mediated by a surface-state band
journal, December 1999

Linear Model Selection by Cross-validation
journal, June 1993

Superstructures of Se adsorbates on Au(111): Scanning tunneling microscopy and spectroscopy study
journal, July 2019

Formation of Two-Dimensional Copper Selenide on Cu(111) at Very Low Selenium Coverage
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Identification of an AgS2 Complex on Ag(110)
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Comparison of S-adsorption on (111) and (100) facets of Cu nanoclusters
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Self-Assembled Selenium Monolayers: From Nanotechnology to Materials Science and Adaptive Catalysis
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Au(111) surface structures induced by adsorption: LEED I(E) analysis of (1×1) and (5×5) Au(111)–S phases
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Coverage Effects and the Nature of the Metal−Sulfur Bond in S/Au(111): High-Resolution Photoemission and Density-Functional Studies
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Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)]
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Zur Thermodynamik von Schwefeldampf
journal, August 1967

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Stabilization of X–Au–X Complexes on the Au(111) Surface: A Theoretical Investigation and Comparison of X = S, Cl, CH ₃ S, and SiH ₃ S
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