Accelerated coarsening of Ag adatom islands on Ag(111) due to trace amounts of S: Mass-transport mediated by Ag-S complexes

Mingmin Shen; Da Jiang Liu; C. J. Jenks; P. A. Thiel; J. W. Evans

doi:10.1063/1.3078033

Accelerated coarsening of Ag adatom islands on Ag(111) due to trace amounts of S: Mass-transport mediated by Ag-S complexes

Mingmin Shen, Da Jiang Liu, C. J. Jenks, P. A. Thiel, J. W. Evans

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Abstract

Scanning tunneling microscopy studies reveal that trace amounts of adsorbed S below a critical coverage on the order of 10 mML have little effect on the coarsening and decay of monolayer Ag adatom islands on Ag(111) at 300 K. In contrast, above this critical coverage, decay is greatly accelerated. This critical value appears to be determined by whether all S can be accommodated at step edges. Accelerated coarsening derives from the feature that the excess S (above that incorporated at steps) produces significant populations on the terraces of metal-sulfur complexes, which are stabilized by strong Ag-S bonding. These include Ag S₂, Ag₂ S₂, Ag₂ S₃, and Ag₃ S₃. Such complexes are sufficiently populous and mobile that they can potentially lead to greatly enhanced metal mass transport across the surface. This picture is supported by density functional theory analysis of the relevant energetics, as well as by reaction-diffusion equation modeling to assess the mechanism and degree of enhanced coarsening.

Original language	English
Article number	094701
Journal	Journal of Chemical Physics
Volume	130
Issue number	9
DOIs	https://doi.org/10.1063/1.3078033
State	Published - 2009
Externally published	Yes

Funding

We thank Karina Morgenstern for information on previous studies of Ag adatom island decay on S-free Ag(111). This work was supported by NSF Grant No. CHE-0809472. D.J.L. was supported by the Division of Chemical Sciences, BES, U.S. Department of Energy (U.S. DOE). This work was performed at Ames Laboratory, which is operated for the U.S. DOE by Iowa State University under Contract No. DE-AC02-07CH11358.

Funders	Funder number
Division of Chemical Sciences
National Science Foundation	0809472
U.S. Department of Energy
Basic Energy Sciences
Iowa State University

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abstract = "Scanning tunneling microscopy studies reveal that trace amounts of adsorbed S below a critical coverage on the order of 10 mML have little effect on the coarsening and decay of monolayer Ag adatom islands on Ag(111) at 300 K. In contrast, above this critical coverage, decay is greatly accelerated. This critical value appears to be determined by whether all S can be accommodated at step edges. Accelerated coarsening derives from the feature that the excess S (above that incorporated at steps) produces significant populations on the terraces of metal-sulfur complexes, which are stabilized by strong Ag-S bonding. These include Ag S2, Ag2 S2, Ag2 S3, and Ag3 S3. Such complexes are sufficiently populous and mobile that they can potentially lead to greatly enhanced metal mass transport across the surface. This picture is supported by density functional theory analysis of the relevant energetics, as well as by reaction-diffusion equation modeling to assess the mechanism and degree of enhanced coarsening.",

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AU - Thiel, P. A.

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AB - Scanning tunneling microscopy studies reveal that trace amounts of adsorbed S below a critical coverage on the order of 10 mML have little effect on the coarsening and decay of monolayer Ag adatom islands on Ag(111) at 300 K. In contrast, above this critical coverage, decay is greatly accelerated. This critical value appears to be determined by whether all S can be accommodated at step edges. Accelerated coarsening derives from the feature that the excess S (above that incorporated at steps) produces significant populations on the terraces of metal-sulfur complexes, which are stabilized by strong Ag-S bonding. These include Ag S2, Ag2 S2, Ag2 S3, and Ag3 S3. Such complexes are sufficiently populous and mobile that they can potentially lead to greatly enhanced metal mass transport across the surface. This picture is supported by density functional theory analysis of the relevant energetics, as well as by reaction-diffusion equation modeling to assess the mechanism and degree of enhanced coarsening.

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Accelerated coarsening of Ag adatom islands on Ag(111) due to trace amounts of S: Mass-transport mediated by Ag-S complexes

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