Structural and electronic properties of atomic oxygen adsorption on Cu(111) surface:A first-principles investigation  

作　　者：MA LiangCai ZHANG JianMin XU KeWei 

机构地区：[1]College of Physics and Information Technology,Shaanxi Normal University [2]School of Physics and Electrical Information Engineering,Ningxia University [3]State Key Laboratory for Mechanical Behavior of Materials,Xi'an Jiaotong University

出　　处：《Science China Chemistry》2013年第3期573-580,共8页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China (Grant No. 51071098);the State Key Development for Basic Research of China (Grant No. 2010CB631002)

摘　　要：By using the first-principles calculations,we have systematically investigated the adsorption of atomic oxygen on Cu(111) surface for a wide range of coverages Θ(from 0.11 to 1.00 ML) and adsorption sites.We found that the fcc-hollow site is the most stable site for oxygen adsorption.The adsorption energy decreases with increasing oxygen coverage due to the increasing repulsive interaction in the overlayer O adatoms.Except for coverage of 1.00 ML,the oxygen-induced lateral relaxations and bucklings are found in the outermost three Cu layers,and the hillock-like as well as ridge-like bucklings are also found for Θ=0.25 ML and Θ=0.75 ML as well as Θ=0.50 ML,respectively.With an increasing oxygen coverage,the work function increases and the surface dipole moment decreases.Electron transfer from the first layer Cu atoms to O adatoms indicates the O-Cu bond having some degree of ionic character,while the hybridization between O 2p and Cu 3d orbitals implies that it also has some degree of covalence character.Moreover,with the increasing oxygen coverage,more Cu 3d and O 2p states are empty thus weakening the binding of O/Cu(111) system,but increase in the PDOS at the Fermi level.This implies an enhancement in the metallic character of the O/Cu(111) system.By using the first-principles calculations, we have systematically investigated the adsorption of atomic oxygen on Cu（111） surface for a wide range of coverages （from 0.11 to 1.00 ML） and adsorption sites. We found that the fcc-hollow site is the most stable site for oxygen adsorption. The adsorption energy decreases with increasing oxygen coverage due to the increasing repulsive interaction in the overlayer O adatoms. Except for coverage of 1.00 ML, the oxygen-induced lateral relaxations and bucklings are found in the outermost three Cu layers, and the hillock-like as well as ridge-like bucklings are also found for =0.25 ML and =0.75 ML as well as =0.50 ML, respectively. With an increasing oxygen coverage, the work function in- creases and the surface dipole moment decreases. Electron transfer from the first layer Cu atoms to O adatoms indicates the O--Cu bond having some degree of ionic character, while the hybridization between O 2p and Cu 3d orbitals implies that it also has some degree of covalence character. Moreover, with the increasing oxygen coverage, more Cu 3d and O 2p states are empty thus weakening the binding of O/Cu（111） system, but increase in the PDOS at the Fermi level. This implies an en- hancement in the metallic character of the O/Cu（111） system.

关 键 词：ADSORPTION OXYGEN RELAXATION electronic structures first-principles calculation 

分 类 号：O562.1[理学—原子与分子物理] TM912[理学—物理]