title: Layer and orientation resolved bond relaxation and quantum entrapment of charge and energy at Be surfaces.
abstract: The chemistry and physics of under-coordination at a surface, which determines the process of catalytic reactions and growth nucleation, is indeed fascinating. However, extracting quantitative information regarding the coordination-resolved surface relaxation, binding energy, and the energetic behavior of electrons localized in the surface skin from photoelectron emission has long been a great challenge, although the surface-induced core level shifts of materials have been intensively investigated. Here we show that a combination of the theories of tight binding and bond order-length-strength (BOLS) correlation [C. Q. Sun, Prog. Solid State Chem., 2007, 35, 1-159], and X-ray photoelectron spectroscopy (XPS) has enabled us to derive quantitative information, by analyzing the Be 1s energy shift of Be(0001), (1010), and (1120) surfaces, for demonstration, regarding: (i) the 1s energy level of an isolated Be atom (106.416 ± 0.004 eV) and its bulk shift (4.694 eV); (ii) the layer- and orientation-resolved effective atomic coordination (3.5, 3.1, 2.98 for the first layer of the three respective orientations), local bond strain (up to 19%), charge density (133%), quantum trap depth (110%), binding energy density (230%), and atomic cohesive energy (70%) of Be surface skins up to four atomic layers in depth. It is affirmed that the shorter and stronger bonds between under-coordinated atoms perturb the Hamiltonian and hence the fascinating localization and densification of surface electrons. The developed approach can be applied to other low-dimensional systems containing a high fraction of under-coordinated atoms such as adatoms, atomic defects, terrace edges, and nanostructures to gain quantitative information and deeper insight into their properties and processes due to the effect of coordination imperfection.
authors: School of Information and Electronic Engineering, Hunan University of Science and Technology, Xiangtan 411201, China.
authors: Yan
authors: Y
authors: Wang
authors: Yan Guang
authors: YG
authors: Nie
authors: Ji Sheng
authors: JS
authors: Pan
authors: Likun
authors: L
authors: Pan
authors: Zhuo
authors: Z
authors: Sun
authors: Chang Q
authors: CQ
authors: Sun