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Enhanced Nanostructure Dynamics on Au(111) with Adsorbed Sulfur due to Au–S Complex Formation

Journal Article · · ChemPhysChem
 [1];  [2];  [3];  [4];  [3]
  1. Iowa State Univ., Ames, IA (United States)
  2. Ames Lab., Ames, IA (United States)
  3. Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
  4. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
+ Show Author Affiliations
Chemisorbed species can enhance the fluxional dynamics of nanostructured metal surfaces which has implications for applications such as catalysis. Scanning tunneling microscopy studies at room temperature reveal that the presence of adsorbed sulfur (S) greatly enhances the decay rate of 2D Au islands in the vicinity of extended step edges on Au(111). This enhancement is already significant at S coverages, θS, of a few hundredths of a monolayer (ML), and is most pronounced for 0.1–0.3 ML where the decay rate is increased by a factor of around 30. For θS close to saturation at about 0.6 ML, sulfur induces pitting and reconstruction of the entire surface, and Au islands are stabilized. Enhanced coarsening at lower θS is attributed to the formation and diffusion across terraces of Au–S complexes, particularly AuS2 and Au4S4, with some lesser contribution from Au3S4. This picture is supported by density functional theory analysis of complex formation energies and diffusion barriers.
Research Organization:
Ames Laboratory (AMES), Ames, IA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-05CH11231; AC02-07CH11358
OSTI ID:
1764843
Alternate ID(s):
OSTI ID: 1804566
Report Number(s):
IS--J-10,339
Journal Information:
ChemPhysChem, Journal Name: ChemPhysChem Journal Issue: 4 Vol. 22; ISSN 1439-4235
Publisher:
ChemPubSoc EuropeCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
density functional calculations
gold
nanostructures
scanning probe microscopy
surface chemistry