Self-organization of S adatoms on Au(111): √3R30° rows at low coverage
Abstract
Using scanning tunneling microscopy, we observe an adlayer structure that is dominated by short rows of S atoms, on unreconstructed regions of a Au(111) surface. This structure forms upon adsorption of low S coverage (less than 0.1 monolayer) on a fully reconstructed cleansurface at 300 K, then cooling to 5 K for observation. The rows adopt one of three orientations that are rotated by 30° from the close-packed directions of the Au(111) substrate, and adjacent S atoms in the rows are separated by √3 times the surface lattice constant, a. Monte Carlo simulations are performed on lattice-gas models, we derived using a limited cluster expansion based on density functional theory energetics. Furthermore, models which include long-range pairwise interactions (extending to 5a), plus selected trio interactions, successfully reproduce the linear rows of S atoms at reasonable temperatures.
- Authors:
-
- Iowa State Univ., Ames, IA (United States)
- Ames Lab., Ames, IA (United States)
- RIKEN Surface and Interface Science Lab., Saitama (Japan)
- Ames Lab. (AMES), Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
- Iowa State Univ., Ames, IA (United States); Ames Lab. (AMES), Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1227393
- Grant/Contract Number:
- CHE1111500; AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 143; Journal Issue: 1; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Walen, Holly, Liu, Da -Jiang, Oh, Junepyo, Lim, Hyunseob, Evans, J. W., Kim, Yousoo, and Thiel, P. A. Self-organization of S adatoms on Au(111): √3R30° rows at low coverage. United States: N. p., 2015.
Web. doi:10.1063/1.4922929.
Walen, Holly, Liu, Da -Jiang, Oh, Junepyo, Lim, Hyunseob, Evans, J. W., Kim, Yousoo, & Thiel, P. A. Self-organization of S adatoms on Au(111): √3R30° rows at low coverage. United States. https://doi.org/10.1063/1.4922929
Walen, Holly, Liu, Da -Jiang, Oh, Junepyo, Lim, Hyunseob, Evans, J. W., Kim, Yousoo, and Thiel, P. A. Mon .
"Self-organization of S adatoms on Au(111): √3R30° rows at low coverage". United States. https://doi.org/10.1063/1.4922929. https://www.osti.gov/servlets/purl/1227393.
@article{osti_1227393,
title = {Self-organization of S adatoms on Au(111): √3R30° rows at low coverage},
author = {Walen, Holly and Liu, Da -Jiang and Oh, Junepyo and Lim, Hyunseob and Evans, J. W. and Kim, Yousoo and Thiel, P. A.},
abstractNote = {Using scanning tunneling microscopy, we observe an adlayer structure that is dominated by short rows of S atoms, on unreconstructed regions of a Au(111) surface. This structure forms upon adsorption of low S coverage (less than 0.1 monolayer) on a fully reconstructed cleansurface at 300 K, then cooling to 5 K for observation. The rows adopt one of three orientations that are rotated by 30° from the close-packed directions of the Au(111) substrate, and adjacent S atoms in the rows are separated by √3 times the surface lattice constant, a. Monte Carlo simulations are performed on lattice-gas models, we derived using a limited cluster expansion based on density functional theory energetics. Furthermore, models which include long-range pairwise interactions (extending to 5a), plus selected trio interactions, successfully reproduce the linear rows of S atoms at reasonable temperatures.},
doi = {10.1063/1.4922929},
journal = {Journal of Chemical Physics},
number = 1,
volume = 143,
place = {United States},
year = {Mon Jul 06 00:00:00 EDT 2015},
month = {Mon Jul 06 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Ab initio phase diagram of oxygen adsorption on W(110)
journal, March 2009
- Stöhr, M.; Podloucky, R.; Müller, S.
- Journal of Physics: Condensed Matter, Vol. 21, Issue 13
Performance of Cluster Expansions of Coverage-Dependent Adsorption of Atomic Oxygen on Pt(111)
journal, December 2011
- Schmidt, David J.; Chen, Wei; Wolverton, C.
- Journal of Chemical Theory and Computation, Vol. 8, Issue 1
The Structure of Atomic Sulfur Phases on Au(111)
journal, June 2007
- Yu, Miao; Ascolani, H.; Zampieri, G.
- The Journal of Physical Chemistry C, Vol. 111, Issue 29
Long-Range Periodicity of S/Au(111) Structures at Low and Intermediate Coverages
journal, December 2013
- Abufager, P. N.; Zampieri, G.; Reuter, K.
- The Journal of Physical Chemistry C, Vol. 118, Issue 1
A sensitive resonance light scattering spectrometry of trace Hg2+ with sulfur ion modified gold nanoparticles
journal, October 2009
- Fan, Ya; Long, Yun Fei; Li, Yuan Fang
- Analytica Chimica Acta, Vol. 653, Issue 2
Multisite lateral interactions and their consequences
journal, November 1991
- Einstein, Theodore L.
- Langmuir, Vol. 7, Issue 11
Real-Time Ab Initio KMC Simulation of the Self-Assembly and Sintering of Bimetallic Epitaxial Nanoclusters: Au + Ag on Ag(100)
journal, June 2014
- Han, Yong; Liu, Da-Jiang; Evans, James W.
- Nano Letters, Vol. 14, Issue 8
Thiobis(hexamethyldisilazane) as a new precursor for the deposition of sulfur on gold: A one-step concerted adsorption process
journal, June 2014
- Koczkur, Kallum M.; Houmam, Abdelaziz
- Surface Science, Vol. 624
Promotion by sulfur of gold catalysts for crotyl alcohol formation from crotonaldehyde hydrogenation
journal, January 1999
- Bailie, Jillian E.; Hutchings, Graham J.
- Chemical Communications, Issue 21
Investigations on Silver Sulfide
journal, October 1953
- Wagner, Carl
- The Journal of Chemical Physics, Vol. 21, Issue 10
Submonolayer Growth with Repulsive Impurities: Island Density Scaling with Anomalous Diffusion
journal, May 1995
- Liu, Shudun; Bönig, Lutz; Detch, John
- Physical Review Letters, Vol. 74, Issue 22
Quantitative Determination of Adsorbate-Adsorbate Interactions
journal, December 1999
- Österlund, L.; Pedersen, M. Ø.; Stensgaard, I.
- Physical Review Letters, Vol. 83, Issue 23
Au(111) surface structures induced by adsorption: LEED I(E) analysis of (1×1) and (5×5) Au(111)–S phases
journal, April 2013
- McGuirk, G. M.; Shin, H.; Caragiu, M.
- Surface Science, Vol. 610
Scanning Tunneling Microscopy Observation of Sulfur Adsorbates on Au(111) at Liquid Nitrogen Temperature
journal, August 2009
- Kurokawa, Shu; Miyawaki, Yuu; Sakai, Akira
- Japanese Journal of Applied Physics, Vol. 48, Issue 8
Coverage Effects and the Nature of the Metal−Sulfur Bond in S/Au(111): High-Resolution Photoemission and Density-Functional Studies
journal, January 2003
- Rodriguez, José A.; Dvorak, Joseph; Jirsak, Tomas
- Journal of the American Chemical Society, Vol. 125, Issue 1
Sulfur−Substrate Interactions in Spontaneously Formed Sulfur Adlayers on Au(111)
journal, August 2001
- Vericat, C.; Vela, M. E.; Andreasen, G.
- Langmuir, Vol. 17, Issue 16
Self-assembled monolayers of thiols and dithiols on gold: new challenges for a well-known system
journal, January 2010
- Vericat, C.; Vela, M. E.; Benitez, G.
- Chemical Society Reviews, Vol. 39, Issue 5
The Chemistry of the Sulfur–Gold Interface: In Search of a Unified Model
journal, March 2012
- Pensa, Evangelina; Cortés, Emiliano; Corthey, Gastón
- Accounts of Chemical Research, Vol. 45, Issue 8
Density functional analysis of key energetics in metal homoepitaxy: Quantum size effects in periodic slab calculations
journal, January 2010
- Liu, Da-Jiang
- Physical Review B, Vol. 81, Issue 3
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Pair- and many-atom interactions in the cohesion of surface clusters: and on W(110)
journal, August 1999
- Koh, Seong Jin; Ehrlich, Gert
- Physical Review B, Vol. 60, Issue 8
Long-ranged adsorbate-adsorbate interactions mediated by a surface-state band
journal, December 1999
- Hyldgaard, Per; Persson, Mats
- Journal of Physics: Condensed Matter, Vol. 12, Issue 1
Alloy Catalyst in a Reactive Environment: The Example of Ag-Cu Particles for Ethylene Epoxidation
journal, January 2010
- Piccinin, Simone; Zafeiratos, Spiros; Stampfl, Catherine
- Physical Review Letters, Vol. 104, Issue 3
Novel Self-Organized Structure of a Ag−S Complex on the Ag(111) Surface below Room Temperature
journal, February 2008
- Shen, Mingmin; Liu, Da-Jiang; Jenks, Cynthia J.
- The Journal of Physical Chemistry C, Vol. 112, Issue 11
Communication: Structure, formation, and equilibration of ensembles of Ag-S complexes on an Ag surface
journal, February 2013
- Russell, Selena M.; Kim, Yousoo; Liu, Da-Jiang
- The Journal of Chemical Physics, Vol. 138, Issue 7
Observing surface chemical transformations by atomic-resolution scanning tunneling microscopy: sulfide electrooxidation on gold(111)
journal, May 1992
- Gao, Xiaoping; Zhang, Yun; Weaver, Michael J.
- The Journal of Physical Chemistry, Vol. 96, Issue 11
Response of the Shockley surface state to an external electrical field: A density-functional theory study of Cu(111)
journal, January 2012
- Berland, K.; Einstein, T. L.; Hyldgaard, P.
- Physical Review B, Vol. 85, Issue 3
An STM, AES and LEED study of the segregated sulfur on Pd(111)
journal, June 1996
- Bömermann, J.; Huck, M.; Kuntze, J.
- Surface Science, Vol. 357-358
Low-temperature adsorption of H2S on Ag(111)
journal, September 2010
- Russell, Selena M.; Liu, Da-Jiang; Kawai, Maki
- The Journal of Chemical Physics, Vol. 133, Issue 12
Sulfur dimers adsorbed on Au(111) as building blocks for sulfur octomers formation: A density functional study
journal, July 2014
- Hernandez-Tamargo, Carlos E.; Montero-Alejo, Ana Lilian; Pujals, Daniel Codorniu
- The Journal of Chemical Physics, Vol. 141, Issue 4
Comparison of cluster expansion fitting algorithms for interactions at surfaces
journal, October 2015
- Herder, Laura M.; Bray, Jason M.; Schneider, William F.
- Surface Science, Vol. 640
Spontaneously Formed Sulfur Adlayers on Gold in Electrolyte Solutions: Adsorbed Sulfur or Gold Sulfide?
journal, July 2008
- Lustemberg, P. G.; Vericat, C.; Benitez, G. A.
- The Journal of Physical Chemistry C, Vol. 112, Issue 30
Search for the Structure of a Sulfur-Induced Reconstruction on Cu(111)
journal, August 2014
- Liu, Da-Jiang; Walen, Holly; Oh, Junepyo
- The Journal of Physical Chemistry C, Vol. 118, Issue 50
Density of Configurational States from First-Principles Calculations: The Phase Diagram of Al-Na Surface Alloys
journal, September 2005
- Borg, Mikael; Stampfl, Catherine; Mikkelsen, Anders
- ChemPhysChem, Vol. 6, Issue 9
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
journal, December 2000
- Henkelman, Graeme; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22
Potential dependent adlayer structures of a sulfur-covered Au(111) electrode in alkaline solution: An in situ STM study
journal, February 2008
- Schlaup, C.; Friebel, D.; Broekmann, P.
- Surface Science, Vol. 602, Issue 4
Sulfur-induced mobilization of Au surface atoms on Au(111) studied by real-time STM
journal, April 2007
- Biener, Monika M.; Biener, Juergen; Friend, Cynthia M.
- Surface Science, Vol. 601, Issue 7
complex on Cu(111) as a candidate for mass transport enhancement
journal, January 2015
- Walen, Holly; Liu, Da-Jiang; Oh, Junepyo
- Physical Review B, Vol. 91, Issue 4
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Theory and Application for the Scanning Tunneling Microscope
journal, June 1983
- Tersoff, J.; Hamann, D. R.
- Physical Review Letters, Vol. 50, Issue 25
Scanning tunneling microscopy observations on the reconstructed Au(111) surface: Atomic structure, long-range superstructure, rotational domains, and surface defects
journal, November 1990
- Barth, J. V.; Brune, H.; Ertl, G.
- Physical Review B, Vol. 42, Issue 15
Determination of atom positions at stacking-fault dislocations on Au(111) by scanning tunneling microscopy
journal, April 1989
- Wöll, Ch.; Chiang, S.; Wilson, R. J.
- Physical Review B, Vol. 39, Issue 11
Observation of a Soliton Reconstruction of Au(111) by High-Resolution Helium-Atom Diffraction
journal, June 1985
- Harten, U.; Lahee, A. M.; Toennies, J. Peter
- Physical Review Letters, Vol. 54, Issue 24
Low-temperature structure of S/Cu(111)
journal, September 2001
- Wahlström, Erik; Ekvall, Inger; Kihlgren, Theresa
- Physical Review B, Vol. 64, Issue 15
Observation of ordered structures for S/Cu(111) at low temperature and coverage
journal, October 1999
- Wahlström, Erik; Ekvall, Inger; Olin, Håkan
- Physical Review B, Vol. 60, Issue 15
Triplet interactions and the c(2×2) overlayer phase diagram
journal, February 1993
- Ceder, G.; Dreyssé, H.; de Fontaine, D.
- Physica A: Statistical Mechanics and its Applications, Vol. 193, Issue 1
First-Principles Theory of Surface Thermodynamics and Kinetics
journal, October 1999
- Stampfl, C.; Kreuzer, H. J.; Payne, S. H.
- Physical Review Letters, Vol. 83, Issue 15
Extended lattice gas interactions of Cu on Cu(111) and Cu(001): Ab initio evaluation and implications
journal, March 2006
- Stasevich, T. J.; Einstein, T. L.; Stolbov, Sergey
- Physical Review B, Vol. 73, Issue 11
Accuracy of first-principles lateral interactions: Oxygen at Pd(100)
journal, June 2007
- Zhang, Yongsheng; Blum, Volker; Reuter, Karsten
- Physical Review B, Vol. 75, Issue 23
Predicting order-disorder phase transitions of O/Pd(111) from ab initio Wang-Landau Monte Carlo calculations
journal, April 2010
- Piccinin, S.; Stampfl, C.
- Physical Review B, Vol. 81, Issue 15
Correlating Josephson supercurrents and Shiba states in quantum spins unconventionally coupled to superconductors
journal, February 2021
- Küster, Felix; Montero, Ana M.; Guimarães, Filipe S. M.
- Nature Communications, Vol. 12, Issue 1
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
First-principles theory of surface thermodynamics and kinetics
other, January 1999
- Stampfl, C.; Kreuzer, H. J.; Payne, S. H.
- College Park, MD : American Physical Society
Response of the Shockley surface state to an external electrical field: A density-functional theory study of Cu(111)
text, January 2011
- Berland, K.; Einstein, T. L.; Hyldgaard, P.
- arXiv
Works referencing / citing this record:
Gold adatoms modulate sulfur adsorption on gold
journal, January 2019
- Carro, Pilar; Salvarezza, Roberto C.
- Nanoscale, Vol. 11, Issue 41
Adsorption of Te atoms on Au(1 1 1) and the emergence of an adatom-induced bound state
journal, February 2017
- Schouteden, Koen; Debehets, Jolien; Muzychenko, Dmitry
- Journal of Physics: Condensed Matter, Vol. 29, Issue 12
Sulfur-driven switching of the Ullmann coupling on Au(111)
journal, January 2018
- Rodríguez-Fernández, Jonathan; Schmidt, Søren Birthin; Lauritsen, Jeppe V.
- Chemical Communications, Vol. 54, Issue 29
Oxygen and sulfur adsorption on vicinal surfaces of copper and silver: Preferred adsorption sites
journal, March 2018
- Liu, Da-Jiang; Thiel, Patricia A.
- The Journal of Chemical Physics, Vol. 148, Issue 12
One-dimensional phosphorus chain and two-dimensional blue phosphorene grown on Au(111) by molecular-beam epitaxy
text, January 2017
- Xu, Jin-Peng; Zhang, Jun-Qiu; Tian, Hao
- arXiv