氯在Au(111)上的吸附：氯覆盖层还是表面氯化物？

Chlorine adsorption on Au(111): chlorine overlayer or surface chloride?

作者信息

Gao Weiwei, Baker Thomas A, Zhou Ling, Pinnaduwage Dilini S, Kaxiras Efthimios, Friend Cynthia M

机构信息

Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford Street, Cambridge, Massachusetts 02138, USA.

出版信息

J Am Chem Soc. 2008 Mar 19;130(11):3560-5. doi: 10.1021/ja077989a. Epub 2008 Feb 22.

DOI:10.1021/ja077989a

PMID:18290645

Abstract

We report the first scanning tunneling microscope (STM) investigation, combined with density functional theory calculations, to resolve controversy regarding the bonding and structure of chlorine adsorbed on Au(111). STM experiments are carried out at 120 K to overcome instability caused by mobile species upon chlorine adsorption at room temperature. Chlorine adsorption initially lifts the herringbone reconstruction. At low coverages (<0.33 ML), chlorine binds to the top of Au(111)-(1 x 1) surface and leads to formation of an overlayer with (square root(3) x square root(3))R30 degree structure at 0.33 ML. At higher coverages, packing chlorine into an overlayer structure is no longer favored. Gold atoms incorporate into a complex superlattice of a Au-Cl surface compound.

摘要

我们报告了首次结合密度泛函理论计算的扫描隧道显微镜（STM）研究，以解决关于氯吸附在Au(111)上的键合和结构的争议。STM实验在120 K下进行，以克服室温下氯吸附时移动物种引起的不稳定性。氯吸附最初会解除人字形重构。在低覆盖度（<0.33 ML）下，氯结合到Au(111)-(1×1)表面的顶部，并在0.33 ML时导致形成具有（√3×√3）R30°结构的覆盖层。在较高覆盖度下，将氯堆积成覆盖层结构不再有利。金原子融入Au-Cl表面化合物的复杂超晶格中。