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Structure of incommensurate gold sulfide monolayer on Au(111)

Journal Article · · Journal of Physical Chemistry
OSTI ID:928179
Two-dimensional confined systems, such as substrate-supported incommensurate layers, are of interest because their structural and electronic properties may differ from those of bulk materials. While advances in experimental techniques have resulted in the growth of many such interesting systems, progress can often be hampered by the lack of an atomistic-scale understanding of the structure, especially for incommensurate systems. In this work, we develop an atomic-scale model for an ordered incommensurate gold-sulfide (AuS) adlayer that has been previously demonstrated to exist on the Au(111) surface, following sulfur deposition and annealing to 450 K. We introduce theoretical techniques within density functional theory to take into account charge transfer in an incommensurate system and model scanning tunneling microscopy images, which are in good agreement with experiment. Our simulations indicate that this model is remarkably robust. We analyze the nature of bonding in this structure using state-of-the-art Wannier-function based techniques. Our analysis provides a natural explanation for the extraordinary robustness and unusual stoichiometry of this layer. This structure and its chemistry have implications for related S-Au interfaces, such as those in self-assembled monolayers of thiols on Au substrates.
Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA
Sponsoring Organization:
USDOE
DOE Contract Number:
W-7405-ENG-48
OSTI ID:
928179
Report Number(s):
UCRL-JRNL-225086
Journal Information:
Journal of Physical Chemistry, Journal Name: Journal of Physical Chemistry Vol. 127; ISSN JPCHAX; ISSN 0022-3654
Country of Publication:
United States
Language:
English