Campus Units

Chemistry, Materials Science and Engineering, Physics and Astronomy, Ames Laboratory

Document Type

Article

Publication Version

Accepted Manuscript

Publication Date

12-28-2020

Journal or Book Title

ChemPhysChem

DOI

10.1002/cphc.202000884

Abstract

Chemisorbed species can enhance the fluxional dynamics of nanostructured metal surfaces which has implications for applications such as catalysis. STM 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, θ S , 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 θ S 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 θ S is attributed to the formation and diffusion across terraces of Au‐S complexes, particularly AuS 2 and Au 4 S 4 , with some lesser contribution from Au 3 S 4 . This picture is supported by DFT analysis of complex formation energies and diffusion barriers.

Comments

This is the peer-reviewed version of the following article: Evans, James William, Peter M. Spurgeon, Da-Jiang Liu, Theresa L. Windus, and Patricia A. Thiel. "Enhanced nanostructure dynamics on Au (111) with adsorbed S due to Au‐S complex formation." ChemPhysChem (2020), which has been published in final form at DOI: 10.1002/cphc.202000884. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving. Posted with permission.

Copyright Owner

Wiley‐VCH GmbH

Language

en

File Format

application/pdf

Available for download on Tuesday, December 28, 2021

Published Version

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