DFT and Monte Carlo study of the W(001) surface reconstruction

The driving force for the W(001) surface reconstruction and electronic structures of pristine and H-covered W(001) surfaces are studied by means of relativistic DFT calculations. The spin-orbit coupling leads to the splitting of the bands. Adsorbed physical monolayer of hydrogen due to forming adsorption bonds stabilizes the (1 × 1) structure of the H/W(001) surface. The performed calculations have not revealed any substantial nesting of Fermi surface, so do not support the Peierls-like charge-density-wave mechanism of the surface reconstruction. The total energy of the (√2 × √2)R45° W(001) surface structure is found to be lower, by 0.14 eV per atom, than for the (1 × 1 W(001). The dependence of the relative intensity of the characteristic LEED reflection on temperature, obtained with the help of Monte Carlo simulations using the interaction energies estimated from DFT calculations, is in good agreement with available experimental data, thus supporting the concept of the order-disorder type of the transition between the low-temperature ((√2 × √2)R45° and room-temperature (1 × 1) surface structures of W(001).     

Stability and magnetism of ultrathin Cr films on a Fe(001) substrate

Itinerant magnetism of ultrathin epitaxial Cr overlayers on a Fe(001) substrate and their energy stability with respect to Cr-Fe interdiffusion were studied by means of ab initio electronic structure calculations. The latter were based on the tight-binding linear muffin-tin orbital method and the coherent potential approximation. The interdiffusion was simulated by two-dimensional substitutionally disordered Cr-Fe alloys formed within two layers at the Cr/Fe interface. For a 1 monolayer Cr film a tendency to surface alloy formation is found in contrast to a 2 monolayer Cr film which seems to be stable with respect to Fe-Cr intermixing. A comparison of the calculated results to recent experimental data is presented and an interplay between the energy stability and magnetism of the films is pointed out. Presented at the VIII-th Symposium on Surface Physics, Třešt’ Castle, Czech Republic, June 28 – July 2, 1999.     

Electronic structures and magnetism of Fe nanowires on Cu（001） and Ag（O01）： A first-principles study

The electronic structures and magnetism of Fe nanowires along the [110] direction on Cu（001） and Ag（001） [Fe（nw）/Cu（001） and Fe（nw）/Ag（001）] are investigated by using the all-electron full-potential linearized augmented plane wave method in the generalized gradient approximation. It is found that the magnetic moment of Fe atom for the Fe（nw）/Cu（001） is 2.99#B, which is slightly smaller than that （3.02μB） for the Fe（nw）/Ag（001） but much larger than that （2.22μB） for the bcc iron. The great enhancement of magnetic moment in the Fe nanowires can be explained by the Fe d-band narrowing and enhancement of the spin-splitting due to a reduction in coordination number, From the calculated spin-polarized layer-projected density of states, it is found that the Fe 3d-states are strongly hybridized with the adjacent Cu 3d-states in the Fe（nw）/Cu（001）, and there exists a strong hybridization between the Fe sp-and the adjacent Ag 4d-states in the Fe（nw）/Ag（001）.     

A precise first-principles study on the non-existence of ferromagnetism in V monolayer on the Nb(001) surface

We report the non-existence of ferromagnetism in V monolayer on the Nb(0 0 1) surface, based on the result obtained by a precise all-electron full-potential linearized augmented plane wave (FLAPW) method within the generalized gradient approximation (GGA). Precisely calculated total energy displays that the paramagnetic state is more stable than the ferromagnetic one. The calculated density of states reveals the microscopic origin of the non-existence of ferromagnetism in the V/Nb(0 0 1) system. The paramagnetic result of our precise calculation contradicts to those of the recent tight-binding calculation using Hubbard-type Hamiltonian by J. Khalifeh [J. Magn. Magn. Mater. 168 (1997) 25] that predicted magnetism of the V overlayers on the Nb(0 0 1) surface.     

Structure and magnetism of the V/Ta(0 0 1) surface: A DFT calculation

Calculations using the density functional theory, norm-conserving pseudopotentials and the generalized gradient approximation are performed for vanadium (V) and tantalum (Ta) clean surfaces, and the V/Ta(0 0 1) system. Vanadium and Ta(0 0 1) clean surfaces are found to be nonmagnetic with large inward relaxations of 9.81% and 11.19%, respectively, in good agreement with experiment and other calculations. However, we obtained an appreciable magnetic moment of 2.24 μB for the V monolayer in the V/Ta(0 0 1) system. The inward relaxation is reduced to 6.01% for the V overlayer on Ta(0 0 1) as a result of its spin polarization. An induced magnetic moment of 0.41 μB is obtained on the Ta interfacial layer, which is found to be anti-ferromagnetically coupled with the V overlayer and the Ta layers below.     

Epitaxial Fe films on ZnSe(001): effect of the substrate surface reconstruction on the magnetic anisotropy

It is well known that Fe films deposited on a c(2 × 2)-reconstructed ZnSe(001) surface show a strong in-plane uniaxial magnetic anisotropy. Here, the effect of the substrate reconstruction on the magnetic anisotropy of Fe has been studied by in situ Brillouin light scattering. We found that the in-plane uniaxial anisotropy is strongly reduced for Fe films grown on a (1 × 1)-unreconstructed ZnSe substrate while the in-plane biaxial one is nearly unaffected by the substrate reconstruction. Calculations of magnetic anisotropy energies within the framework of ab initio density functional theory reveal that the strong suppression of anisotropy at the (1 × 1) interface occurs due to complex atomic relaxations as well as the competing effects originating from magnetocrystalline anisotropy and dipole-dipole interactions. For both sharp and intermixed c(2 × 2) interfaces, the magnetic anisotropy is enhanced compared to the (1 × 1) case due to the further lowering of symmetry. The theoretical results are in agreement with the experimental findings.     

Local spin density total energy study of surface magnetism: V (100)

Results of self-consistent all-electron local (spin) density functional studies of the electronic and magnetic properties of vanadium (100) 1-, 3-, 5- and 7-layers films are reported using our full-potential linearized augmented plane wave (FLAPW) method. The calculated work function, 4.2 eV, agrees very well with the experimental value of 4.12 eV. From both Stoner factor analyses and spin-polarized total energy calculations, it is concluded that V(100) undergoes a ferromagnetic phase transition only for the monolayer system. The magnetic moment is found to be 3.09μ_B per atom of this monolayer film and to have a total energy 57 mRy below that of the paramagnetic structure. For multilayer V(001) systems, the sharp surface density-of-states peak which is characteristic of the occurrence of surface magnetism in the 3d transition metals is located 0.3 eV above the Fermi level. As a result, the paramagnetic state is stable. In addition, no enhancement of the exchange-correlation integral is found for the surface atoms compared with the bulk value. The lower energy of the paramagnetic structure is further supported by total energy investigations of the multilayer relaxation of V(100) — the calculated interlayer spacings for the paramagnetic surface with a 9% contraction of the topmost interlayer spacing and a 1% expansion of the second interlayer spacing with respect to its bulk value are in good agreement with LEED measurements. It is suggested that the surface magnetism of V(100) may be associated with surface oxygen or caused by impurity induced surface reconstructions.     

Evidence of substrate metallization by Li adsorption on the Si(001) surface

We report an evidence of substrate metallization induced by Li adsorption on the Si(001) surface, based on the combined results of electron energy-loss (EEL) and angle-resolved photoemission (ARP) measurements. The metallic surface at a low dose of Li manifests itself as a loss peak due to an intraband surface plasmon in EEL spectra and a metallic peak in ARP spectra. These peaks are coherently understood in terms of substrate metallization, where electrons from Li adatoms partially occupy the empty substrate surface bands. Furthermore, the unique negative dispersion of the plasmon reveals that local field effects may cause such an anomalous dispersion.     

Lithium intercalation effects on the V2O5 (001) surface

The lithium intercalation effects on the V₂O₅(001) surface have been investigated by means of the LCAO-Hartree–Fock method using various clusters. Considerable charge donated by Li to the host is transferred preferentially to the bridging oxygens rather than to the vanadyl oxygens or metals. A partial reduction of the vanadium center near the lithium is obtained.     

A DFT study of CO adsorbed on clean and hydroxylated anatase TiO2 (001) surfaces

The adsorbate–substrate interaction between carbon monoxide and clean and hydroxylated surfaces of anatase (001) was simulated by periodic DFT calculations. For the clean surface, different periodicities were taken into account in order to investigate the influence of lateral effects. The results show that the molecule interacts only with the penta-coordinated titanium ion when high surface coverages are employed, whereas it interacts with both the titanium and the di-coordinated oxygen ions when the smallest surface coverage is considered. Adsorption on the hydroxylated surface, which was carried out for the first time, was studied by considering the largest used periodicity and focusing attention on the influence of both the terminal and bridging OH groups. The resulting data show that, in the case of adsorption on the hydroxylated surface, no additional bond between the surface oxygen and the carbon atom is present. Therefore, in a regime of very low surface coverage, the molecule behaves in a very different way when it interacts with a clean or a hydroxylated surface.     

Indenter size effect on the reversible incipient plasticity of Al(001) surface:Quasicontinuum study

Indenter size effect on the reversible incipient plasticity of Al(001) surface is studied by quasicontinuum simulations.Results show that the incipient plasticity under small indenter, the radius of which is less than ten nanometers, is dominated by a simple planar fault defect that can be fully removed after withdrawal of the indenter; otherwise, irreversible incipient plastic deformation driven by a complex dislocation activity is preferred, and the debris of deformation twins, dislocations,and stacking fault ribbons still remain beneath the surface when the indenter has been completely retracted. Based on stress distributions calculated at an atomic level, the reason why the dislocation burst instead of a simple fault ribbon is observed under a large indenter is the release of the intensely accumulated shear stress. Finally, the critical load analysis implies that there exists a reversible-irreversible transition of incipient plasticity induced by indenter size. Our findings provide a further insight into the incipient surface plasticity of face-centered-cubic metals in nano-sized contact issues.     

A periodic DFT study of water and ammonia adsorption on anatase TiO2 (001) slab

Water and ammonia adsorption mechanisms on anatase TiO₂ (001) slab surface are investigated by means of periodic DFT approach. Molecular and dissociative adsorption energies for water are calculated to be ? 15 kcal/mol and ? 32 kcal/mol, respectively. Similarly, molecular and dissociative adsorption energies of ammonia on the same surface are found as ? 25 kcal/mol and ? 20 kcal/mol. A reverse result in this order is reached for the previous case of ONIOM cluster study (? 23 kcal/mol and ? 37 kcal/mol, respectively). The vibration frequency values are computed for the optimized geometries of adsorbed water and ammonia molecules on anatase TiO₂ (001) slab surface and compared with the values reported in the literature.     

氢吸附金刚石（001）表面的第一性原理研究

采用第一性原理方法研究氢吸附的金刚石（001）表面，计算了氢吸附金刚石表面构型.通过分析吸附前后空间电荷分布的变化，发现吸附H原子的金刚石（001）表面电荷向H原子转移，即表明氢吸附的金刚石表面带负电.分析了这种现象的微观机制，以及它对金刚石表面电学性质的影响. 关键词： 第一性原理计算 金刚石（001）面 表面吸附 电荷密度分布     

AB initio hartree-fock study of the MgO(001) surface

The MgO(001) surface has been studied with an ab initio Hartree-Fock crystalline orbital LCAO program. An optimized basis set containing nine atomic orbitals (three s and six p) per atom has been used. The semi-infinite crystal has been simulated by a slab containing three planes (six atoms per cell). In agreement with the most recent LEED experiments, no relaxation is found and the “rumpling” is very small (1% of the nearest neighbour separation in the bulk). The analysis of the electron charge distribution and of the ion multipoles shows that the fully ionic character found for the bulk is maintained at the surface, and that the anion deformation is very small. A surface energy of 1.43 J/m² was obtained.     

High performance III/V RTD and PIN diode on a silicon (001) substrate

We report on the fabrication of high performance InP-based devices on an exact (001)Si-substrate. On an InP-on-Si quasi-substrate, the growth of superlattices and low-temperature InAlAs buffer for surface and device layer improvement is investigated. The selected device examples are an InGaAsP PIN diode and an (In)AlAs/In(Ga)As resonant tunnelling diodes. The functionality of these examples relies sensitively on sharp interfaces of ultra thin layers and a high optical quality of epitaxially grown III/V layers silicon substrates. A qualitative improvement is obtained for a low-temperature InAlAs buffer layer grown prior to the of device layers. Based on device models extracted from the fabricated devices a potentially low-cost optical receiver circuit on a Si-substrate is proposed and simulated using HSPICE up to 10 Gbit/s. PACS 73.40.Kp; 73.43.Jn; 73.61.Ey; 78.70.Ck; 78.70.Gq