Adsorption of sulfur on Au(111) surface: An extremely stable configuration

The sulfur adsorption on gold surface is a hot topic in catalysis, electrochemistry and chemical sensors. However, the multiple structures of adsorbed sulfur and sulfur-induced reconstruction in gold substrate topography are still open problems until now. Here we performed an extensively study on sulfur adsorption on Au(111) surface based on First-Principles calculation. Our results show that the sulfur adsorption with additional Au atoms is not favorable. Thus, the well-known lifting of the herringbone reconstruction of Au(111) after sulfur adsorption can't be attributed to the lifting gold atoms. More importantly, we proposed an extremely stable configuration of S-Au(111) surface characterized by (√3 × √3)R30° at 0.33 coverage, in which each S atom is chemisorbed in 3-fold coordinated sites and all the surface-Au atoms are terminated. Finally, the good agreement between our simulated STM and LEED images and experimental observations illuminates the truth that our proposed configuration is also favorable in experiment. This super stable S-adsorbed surface can be used as a starting point for the growth of two dimensional transition metal sulfides.