Size dependence of nanostructures: Impact of bond order deficiency

This chapter provides an overview of quasiparticle calculations in solids, and, in particular, the GW approximation (GWA). A successful approximation for the determination of excited states of solids is based on the quasiparticle concept and the Green function method. The Coulomb repulsion between electrons leads to a depletion of negative charge around a given electron, and the ensemble of this electron and its surrounding positive screening charge forms a quasiparticle. The mathematical description of quasiparticles is based on the single-particle Green function (G), whose exact determination requires complete knowledge of the quasiparticle self-energy ∑. The self-energy ∑ is a non-Hermitian, energy-dependent, nonlocal operator that describes exchange and correlation effects beyond the Hartree approximation. A determination of the self-energy can only be approximate, and a working scheme for the quantitative calculation of excitation energies in metals, semiconductors, and insulators is the so-called dynamically screened interaction or the GWA. The chapter also discusses (1) the physics and extensions of the GWA; (2) numerical aspects of GWA calculations; (3) applications of the GWA to semiconductors, insulators and metals; and (4) the relevance of GWA calculations to optical response. Finally, the chapter presents parallel algorithms both for reciprocal and real-space/imaginary-time GWA calculations and several alternative methods to determine excited states of solids within density functional theory.

Quasiparticle calculations in solids

Auger parameter and Wagner plot in the characterization of chemical states by X-ray photoelectron spectroscopy: a review

Two-dimensional layered MoS2 shows great potential for nanoelectronic and optoelectronic devices due to its high photosensitivity, which is the result of its indirect to direct band gap transition when the bulk dimension is reduced to a single monolayer. Here, we present an exhaustive study of the band alignment and relativistic properties of a van der Waals heterostructure formed between single layers of MoS2 and graphene. A sharp, high-quality MoS2-graphene interface was obtained and characterized by micro-Raman spectroscopy, high-resolution X-ray photoemission spectroscopy (HRXPS), and scanning high-resolution transmission electron microscopy (STEM/HRTEM). Moreover, direct band structure determination of the MoS2/graphene van der Waals heterostructure monolayer was carried out using angle-resolved photoemission spectroscopy (ARPES), shedding light on essential features such as doping, Fermi velocity, hybridization, and band-offset of the low energy electronic dynamics found at the interface. We show th...

Band Alignment and Minigaps in Monolayer MoS2-Graphene van der Waals Heterostructures

The purpose of this article is to provide an overview of the surface structures of the clean surfaces of tetrahedrally coordinated semiconductors within the context of identifying the main features of their structural chemistry. We develop the point of view that the surface regions of these materials form twodimensional (2D) compounds whose bonding is constrained by the requirement of epitaxy with the substrate1 and that the coordination chemistry of these compounds differs from that of molecules or (three-dimensional) bulk solids in specific ways.2 Our coverage is confined to low-index faces. Specifically, our interest lies in the atomic geometries of ideal single-crystal regions of surfaces rather than in the morphology of surfaces with multiple domains, steps, or defects. Finally, although similar considerations have been applied to interpret oxide surface structures more generally,3 our attention herein is confined to tetrahedrally coordinated elemental and binary compound semiconductors. The traditional approach to constructing a review of this type is to consider each surface separately and to describe the structural studies4-11 or theoretical predictions of surface structure4-7,12,13 for each individual surface. This procedure offers an abundance of case histories, but little by way of guidance concerning how to make sense out of the wealth of Dr. Charles B. Duke is Senior Research Fellow at Xerox Corporation. Prior to holding this position, he was Deputy Director and Chief Scientist of the Pacific Northwest Division of the Battelle Memorial Institute and Affiliate Professor of Physics at the University of Washington. From 1972 to 1988 he held various technical and management positions at the Xerox Research Laboratories in Webster, NY and was an Adjunct Professor of Physics at the University of Rochester. During 1969−72, he was a Professor of Physics and member of the Materials Research Laboratory and Coordinated Science Laboratory at the University of Illinois in Urbana, IL, following six years as a staff member of the General Electric Corporate Research and Development Center in Schenectady, NY. He received his Ph.D. in physics from Princeton in 1963 following a B.S. Summa Cum Laude with distinction in mathematics from Duke University in 1959. He is a Fellow and an Honorary Member of the American Vacuum Society, a Fellow of the American Physical Society, a Fellow of the IEEE, and a life member of Sigma Xi. In 1977, Dr. Duke received the Medard W. Welch Award in Vacuum Science and Technology. In 1979 he served as President of the American Vacuum Society, and since 1979, as Treasurer of its Electronic Materials and Processing Division. He served on the Board of Directors of the American Vacuum Society for seven years. He was chairman of the 1977 Gordon Research Conference on the Chemistry and Physics of Solids and of the 1983 Gordon Research Conference on Organic Thin Films and Solid Surfaces. In 1981 he was named one of the ISI 1000 internationally most cited scientists. During 1985−86 he served as founding editor-in-chief of the Journal of Materials Research, the official journal of the Materials Research Society. From 1988 to 1992 and 1995 to 1997, he served (will be serving) on the council of the Materials Research Society, serving as Treasurer during 1991−2. In 1992 he was named editor of Surface Science. In 1993 he was elected to the National Academy of Engineering. He is serving on the Council of the American Physical Society during 1995−8. He was chairman of the Board of Editors of the Journal of Vacuum Science and Technology during 1976−82 and is currently a member of the editorial boards of Journal of Materials Research, Critical Reviews of Solid-State and Materials Sciences, Surface Science Reports, the Chemistry and Physics of Surfaces and Interfaces, and the Encyclopedia of Applied Physics. He served on the Governing Board of the American Institute of Physics from 1976 to 1987, being a member of the Board’s Executive Committee, Corporate Associates Committee, Educational Policy Committee, Journals Committee, and Committee on Public Education and Information. He has written over 350 papers on surface science, materials research, semiconductor physics, and the electronic structure of molecular solids, as well as a monograph on electron tunneling in solids. He is the editor of Surface Science: The First Thirty Years. 1237 Chem. Rev. 1996, 96, 1237−1259

Semiconductor Surface Reconstruction: The Structural Chemistry of Two-Dimensional Surface Compounds.

Extremely well-resolved Si 2p core-level spectra have been obtained from the clean Si(001) surface. Spectra from the cold c(4×2) and the RT 2×1 surfaces are very similar, implying that the local structure of the two reconstructions is the same. Shifted components originating from both up and down atoms of asymmetric dimers, as well as second-layer atoms, are identified. The split of ∼0.55 eV between the two dimer-atom components points to a substantial charge transfer within the dimers. We find no support for the recently proposed crystal-field splitting of the surface components

Core-level spectroscopy of the clean Si(001) surface: Charge transfer within asymmetric dimers of the 2 x 1 and c(4 x 2) reconstructions.

The atomic structures of the low-coverage 2\ifmmode\times\else\texttimes\fi{}2 phases of Al, Ga, and In on Si(100) were determined on the basis of first-principles total-energy calculations and angle-resolved photoemission experiments. The proposed structure consists of rows of ad-dimers, with the ad-dimers oriented parallel to the underlying Si dimers. Angle-resolved photoemission experiments performed for Si(100)2\ifmmode\times\else\texttimes\fi{}2:ln are in good agreement with the calculated surface-state dispersions for the parallel ad-dimer model. The existence of lower coverage 3\ifmmode\times\else\texttimes\fi{}2 and 5\ifmmode\times\else\texttimes\fi{}2 phases results from repulsive interactions between neighboring rows of ad-dimers.

Structure of low-coverage phases of Al, Ga, and In on Si(100)

Atomic origins of the surface components in the Si 2p core-level spectra of the Si(111)7 x 7 surface.

Les resultats des mesures impliquent que la phase monohydrure est formee dans la maille elementaire 7×7 apres exposition a l'hydrogene. On pense, en contradiction avec des travaux anterieurs, que la composante de surface, qui se deplace vers une energie de liaison inferieure, correspond aux atomes au repos et non aux atomes adsorbes

C. J. Karlsson

Papers

Core-level spectroscopy of the clean Si(001) surface: Charge transfer within asymmetric dimers of the 2 x 1 and c(4 x 2) reconstructions.

Structure of low-coverage phases of Al, Ga, and In on Si(100)

Atomic origins of the surface components in the Si 2p core-level spectra of the Si(111)7 x 7 surface.

Hydrogen chemisorption on Si(111)7 x 7 studied with surface-sensitive core-level spectroscopy and angle-resolved photoemission.

Electronic structure of clean and hydrogen-chemisorbed Ge(001) surfaces studied by photoelectron spectroscopy.