Supported magnetic nanoclusters: Softlanding of Pd clusters on a MgO surface

Low-energy deposition of neutral Pd_N clusters (N=2-7 and 13) on a MgO(001) surface F-center (FC) was studied by spin-density-functional molecular dynamics simulations. The incident clusters are steered by an attractive "funnel" created by the FC, resulting in adsorption of the cluster, with one of its atoms bonded atop of the FC. The deposited Pd_2-Pd_6 clusters retain their gas-phase structures, while for N>6 surface-commensurate isomers are energetically more favorable. Adsorbed clusters with N > 3 are found to remain magnetic at the surface.Comment: 5 pages, 2 figs, Phys.Rev.Lett., accepte

Structural models for the Si(553)-Au atomic chain reconstruction

Recent photoemission experiments on the Si(553)-Au reconstruction show a one-dimensional band with a peculiar ~1/4 filling. This band could provide an opportunity for observing large spin-charge separation if electron-electron interactions could be increased. To this end, it is necessary to understand in detail the origin of this surface band. A first step is the determination of the structure of the reconstruction. We present here a study of several structural models using first-principles density functional calculations. Our models are based on a plausible analogy with the similar and better known Si(557)-Au surface, and compared against the sole structure proposed to date for the Si(553)-Au system [Crain JN et al., 2004 Phys. Rev. B 69 125401 ]. Results for the energetics and the band structures are given. Lines for the future investigation are also sketched

Diffusion of Pt dimers on Pt(111)

We report the results of a density-functional study of the diffusion of Pt dimers on the (111) surface of Pt. The calculated activation energy of 0.37 eV is in {\em exact} agreement with the recent experiment of Kyuno {\em et al.} \protect{[}Surf. Sci. {\bf 397}, 191 (1998)\protect{]}. Our calculations establish that the dimers are mobile at temperatures of interest for adatom diffusion, and thus contribute to mass transport. They also indicate that the diffusion path for dimers consists of a sequence of one-atom and (concerted) two-atom jumps.Comment: Pour pages postscript formatted, including one figure; submitted to Physical Review B; other papers of interest can be found at url http://www.centrcn.umontreal.ca/~lewi

Strain-Dependence of Surface Diffusion: Ag on Ag(111) and Pt(111)

Using density-functional theory with the local-density approximation and the generalized gradient approximation we compute the energy barriers for surface diffusion for Ag on Pt(111), Ag on one monolayer of Ag on Pt(111), and Ag on Ag(111). The diffusion barrier for Ag on Ag(111) is found to increase linearly with increasing lattice constant. We also discuss the reconstruction that has been found experimentally when two Ag layers are deposited on Pt(111). Our calculations explain why this strain driven reconstruction occurs only after two Ag layers have been deposited.Comment: 4 pages, 3 figures, Phys. Rev. B 55 (1997), in pres

Projection of plane-wave calculations into atomic orbitals

The projection of the eigenfunctions obtained in standard plane-wave first-principle electronic-structure calculations into atomic-orbital basis sets is proposed as a formal and practical link between the methods based on plane waves and the ones based on atomic orbitals. Given a candidate atomic basis, ({\it i}) its quality is evaluated by its projection into the plane-wave eigenfunctions, ({\it ii}) it is optimized by maximizing that projection, ({\it iii}) the associated tight-binding Hamiltonian and energy bands are obtained, and ({\it iv}) population analysis is performed in a natural way. The proposed method replaces the traditional trial-and-error procedures of finding appropriate atomic bases and the fitting of bands to obtain tight-binding Hamiltonians. Test calculations of some zincblende semiconductors are presented.Comment: RevTex. 4 pages. 3 uuencoded compressed (tared) postscript figs. To appear in Solid St. Commu

A mixed ultrasoft/normconserved pseudopotential scheme

A variant of the Vanderbilt ultrasoft pseudopotential scheme, where the normconservation is released for only one or a few angular channels, is presented. Within this scheme some difficulties of the truly ultrasoft pseudopotentials are overcome without sacrificing the pseudopotential softness. i) Ghost states are easily avoided without including semicore shells. ii) The ultrasoft pseudo-charge-augmentation functions can be made more soft. iii) The number of nonlocal operators is reduced. The scheme will be most useful for transition metals, and the feasibility and accuracy of the scheme is demonstrated for the 4d transition metal rhodium.Comment: 4 pages, 2 figure

Electrons in Dry DNA from Density Functional Calculations

The electronic structure of an infinite poly-guanine - poly-cytosine DNA molecule in its dry A-helix structure is studied by means of density-functional calculations. An extensive study of 30 nucleic base pairs is performed to validate the method. The electronic energy bands of DNA close to the Fermi level are then analyzed in order to clarify the electron transport properties in this particularly simple DNA realization, probably the best suited candidate for conduction. The energy scale found for the relevant band widths, as compared with the energy fluctuations of vibrational or genetic-sequence origin, makes highly implausible the coherent transport of electrons in this system. The possibility of diffusive transport with sub-nanometer mean free paths is, however, still open. Information for model Hamiltonians for conduction is provided.Comment: 8 pages, 4 figure

First principles study of the adsorption of C60 on Si(111)

The adsorption of C60 on Si(111) has been studied by means of first-principles density functional calculations. A 2x2 adatom surface reconstruction was used to simulate the terraces of the 7x7 reconstruction. The structure of several possible adsorption configurations was optimized using the ab initio atomic forces, finding good candidates for two different adsorption states observed experimentally. While the C60 molecule remains closely spherical, the silicon substrate appears quite soft, especially the adatoms, which move substantially to form extra C-Si bonds, at the expense of breaking Si-Si bonds. The structural relaxation has a much larger effect on the adsorption energies, which strongly depend on the adsorption configuration, than on the charge transfer.Comment: 4 pages with 3 postscript figures, to appear in Surf. Science. (proceedings of the European Conference on Surface Science ECOSS-19, Sept 2000

Optical properties of the vibrations in charged C60_{60} molecules

The transition strengths for the four infrared-active vibrations of charged C$_{60}$ molecules are evaluated in self-consistent density functional theory using the local density approximation. The oscillator strengths for the second and fourth modes are strongly enhanced relative to the neutral C$_{60}$ molecule, in good agreement with the experimental observation of ``giant resonances'' for those two modes. Previous theory, based on a ``charged phonon'' model, predicted a quadratic dependence of the oscillator strength on doping, but this is not borne out in our calculations.Comment: 10 pages, RevTeX3.

Surface Magnetic Phase Diagram of Tetragonal Manganites

To gain insights into the fundamental and characteristic features of the surface of doped manganites, we constructed a general magnetic phase diagram of La$_{1-x}$Sr$_{x}$MnO$_3$ (001) surfaces in the plane spanned by $x$ and the bulk tetragonal distortion $c/a$, from the first-principles calculations. We found that the surfaces are quite different from the bulk in the sense that both the (La, Sr)O and MnO$_2$ terminated surfaces show strong tendency toward antiferromagnetism (A-type and C-type respectively). The basic physics governing the phase diagram can be understood in terms of the surface orbital polarizations. It is also found that the strong surface segregation of Sr atoms is mostly caused by the electrostatic interaction and will further enhance the tendency to surface antiferromagnetism.Comment: 3 figure