Surface magnetism during oxygen-aided Fe homoepitaxy

Magnetization-induced optical surface second harmonic generation (SHG) in the longitudinal geometry was used to study magnetism on the p(1 x 1)O/Fe(001) surface during a layer-by-layer Fe growth with surfactant oxygen. Considerable one-monolayer oscillations were observed. Minima of the magnetization-induced contributions to the second order dielectric susceptibility were detected at half-filled monolayers. These contributions were accessed either by measuring a purely magnetic SHG yield, or indirectly from the magnetization dependence of the overall SHG signal, both providing consistent results. The origin of the oscillatory surface magnetism is consistent with the expected oscillating oxygen induced relaxation due to the surface Fe islands.     

Nonlinear optical spectroscopy of suboxides at oxidized Si(111) interfaces

Native oxidation of the Si(111)(1 x 1)H surface causes the appearance and disappearance of second-harmonic generation (SHG) resonances related to specific bonding configurations of Si atoms at the interface. Resonances at 3.52 eV two-photon energy observed in p-polarized SHG spectra are indicative of a Si suboxide configuration present in a partially oxidized Si surface bilayer. Similar resonances are observed in spectra of thermally oxidized Si(111) and point to Si2+ suboxide states at the buried interface.     

Surface plasmon effects on surface second harmonic generation during Au nanoparticle deposition onto H–Si(1 1 1)

Deposition of Au nanoparticles from aqueous HF onto H–Si(1 1 1) was studied in situ by surface second harmonic generation (SHG) and ex situ by extinction spectroscopy and non-contact atomic force microscopy (AFM). AFM measurements indicate that the maximum SHG intensities occur at lateral particle diameters of approximately 90–100 nm independent of solution phase composition, but with an intensity that depends on solution phase composition.

Employing the evolution of SHG intensity to monitor lateral cluster growth, simultaneous Au deposition and Si oxidation exhibit apparent kinetic reaction orders of 1/2 and zero with respect to HF and Au(CN)₂⁻, respectively. These results are similar to those obtained purely from ex situ AFM analysis. The variations in SHG intensity with Au(CN)₂⁻ concentration can be related to particle nucleation densities. These results demonstrate the utility of SHG as an in situ probe of particle growth.     

Asymmetric distribution of surface second harmonic generation for thin silver films deposited on Si(111)

The asymmetric distributions of surface optical second harmonic generation (SHG) through azimuthally angular scans of (111) silicon wafers on which thin silver films were deposited, have been detected with different polarizations of output beams. On account of the inversion symmetry of silicon crystals, the SHG for the Ag/Si system is mainly contributed by the silver film and the silicon surface. In this work, we found that the interface strain implies an asymmetric intensity variation of SHG with respect to the surface azimuthal angles as an ultra thin Ag film is deposited on silicon wafers. This asymmetric behavior is prominent as the deposited silver layer is heated so that the continuous film aggregates to become granular nanoparticles. Similar changes of the surface asymmetric SHG are observed for a bare Si wafer imposed upon by an external force.     

Chlorine adsorption on Si(1 1 1) studied by optical methods

The adsorption process of chlorine on Si(1 1 1) has been studied by means of real time surface differential reflectance (SDR) spectroscopy and second harmonic generation (SHG). The structure observed at 3.6 eV in SDR spectra is attributed to transitions including Si–Cl antibonding states. However, the overall feature is due to the removal of the electronic states of the clean surface. Developments of adsorption on Si adatom dangling bonds and breaking of adatom back bonds are obtained from SDR spectra and second harmonic (SH) intensity. They are well fit by the solutions of the rate equations under the assumption of adsorption of atoms without migration, and the initial sticking probability on the dangling bonds and the initial breaking probability of the back bonds are determined. Dependence of the adsorption kinetics on the carrier concentration is briefly reported.     

Atomic configurations during Si incorporation on GaAs(001) in As atmosphere evidenced by reflectance difference spectroscopy

The structural ordering of surface atoms during Si deposition on singular and vicinal GaAs(001) surfaces has been studied by reflectance difference (RD) spectroscopy using the difference function between the Si-covered and the bare surface. In dependence on the Si coverage the difference spectra correspond to RD spectra of the bare Si(001)-(1×2) or of the As-terminated Si(001):As(2×1) surface. This finding and the behaviour of RD transients recorded at 3.8 eV photon energy allows to define a (3×2)α phase with Si dimers in the top layer and Ga dimers in the third layer, and a (3×2)β phase with As-dimer rows on top of Si in the second layer.     

Changes of phase and intensity of optical SHG with Ag deposition on Si(111)-7×7 surfaces

The phase and intensity of optical second harmonic generation (SHG) were studied in Ag deposition on the Si(1 1 1) surfaces. The 7×7 reconstruction of the surface changed to the 1×1 structure in room temperature deposition. The SHG intensity reduced and the phase shifted to +180° with this structural change. Meanwhile, the 7×7 reconstruction changed to the reconstruction in 400 °C deposition. With this structural change, the SHG intensity increased and the phase shifted to −250°. An analysis with anharmonic oscillator model showed that the changes in room temperature deposition were due to the quenching of the surface dangling bond states of the 7×7 reconstruction by the Ag deposition, whereas those in 400 °C deposition were due to the appearance of new surface states of the reconstruction.     

Single-beam and enhanced two-beam second-harmonic generation from silicon nanocrystals by use of spatially inhomogeneous femtosecond pulses

Optical second-harmonic generation (SHG) is used as a noninvasive probe of the interfaces of Si nanocrystals (NCs) embedded uniformly in an SiO2 matrix. Measurements of the generated SH mode verify that the second-harmonic polarization has a nonlocal dipole form proportional to (E x Delta inverted) E that depends on inhomogeneities in the incident field E, as proposed in recent models based on a locally noncentrosymmetric dipolar response averaged over the spherical NC interfaces. A two-beam SHG geometry is found to enhance this polarization greatly compared to single-beam SHG, yielding strong signals useful for scanning, spectroscopy, and real-time monitoring. This configuration provides a general strategy for enhancing the second-order nonlinear response of centrosymmetric samples, as demonstrated here for both Si nanocomposites and their glass substrates.     

β-SiC(001)-(2×1)表面结构的第一性原理研究

利用缀加平面波加局域轨道(APW+LO)的第一性原理方法计算了β-SiC(001)-(2×1)表面的原子及电子结构. 原子结构的计算结果表明，与Si(001)-(2×1) 表面的非对称性Si二聚体模型不同，β-SiC(001)-(2×1)表面为对称性的Si二聚体模型，其二聚体的Si原子间键长也较大，为0.269nm. 电子结构的计算结果表明，在费米能级处有明显的态密度，因此β-SiC(001)-(2×1)表面呈金属性. 在带隙附近存在四个表面态带,其中的两个占有表面态带已由价带的同步辐射光电子能谱实验得到证实. 关键词： 碳化硅 缀加平面波加局域轨道方法 原子结构 电子结构     

Optical studies of Si/SiO<Subscript><Emphasis Type="Bold">2</Emphasis></Subscript> interfaces by second-harmonic generation spectroscopy of silicon interband transitions

Optical second-harmonic generation (SHG) studies of Si/SiO₂ interfaces by resonant two-photon excitation of Si interband transitions are reviewed. Three different types of interband resonances at Si interfaces are identified in SHG spectra: (i) E₁ and E₂ critical-point bulk interband transitions in the space-charge region of charged Si interfaces, (ii) E₁- and E₂-type transitions associated with Si atoms at the interface in bulk-like tetrahedral coordination, and (iii) transitions related to Si interface atoms with bonding properties specific of the atomic structure of the interface. The effects of the polarity of space-charge fields on SHG spectra of Si(100)/SiO₂ interfaces are also discussed. PACS 73.40.Qv; 73.20.-r; 42.65.Ky     

K-induced surface structural change of Si(1 1 1)-7 × 7 probed by second-harmonic generation

The growth of thin K films on Si(1 1 1)-7 × 7 has been investigated by selecting the input and output polarizations of second-harmonic generation (SHG) at room temperature (RT) and at an elevated temperature of 350 °C. The SH intensity at 350 °C showed a monotonic increase with K coverages up to a saturated level, where low energy electron diffraction (LEED) showed a 3 × 1 reconstructed structure. The additional deposition onto the K-saturated surface at 350 °C showed only a marginal change in the SH intensity. These variations are different from the multi-component variations up to 1 ML and orders of magnitude increase due to excitation of plasmons in the multilayers at RT. The variations of SHG during desorption of K at 350 °C showed a two-step decay with a marked shoulder which most likely corresponds to the saturation K coverage of the Si(1 1 1)-3 × 1-K surface. The dominant tensor elements contributing to SHG are also identified for each surface.     

原位二次谐波研究Si(111)电极/电解液界面

本文利用电势依赖的原位二次谐波方法(SHG)研究Si(111)电极界面. 研究发现Si(111)电极在不同方位角下,其不同的偏振组合的SHG强度曲线随外加电势的变化呈现直线型或抛物线型两种不同的线型. 这种电势依赖的SHG响应曲线的差别可以用Si(111)电极的各向异性和各向同性对SHG信号的贡献来解释. Si(111)电极的各向异性和各向同性的贡献主要源于Si(111)电极掺杂浓度的增加.     

Nitric acid-stabilized superparamagnetic iron oxide nanoparticles studied with X-rays

Using density functional theory, we systematically investigate the adsorption geometries and electrical properties of (3,3) carbon nanotube (CNT) integrated on hydrogen-terminated Si(001):1?×?1 surface. Prior to adsorption of the CNT, the surface is patterned in two different ways by desorbing selective hydrogen atoms from the surface. The (3,3) CNT which is metallic in nature becomes semiconducting with a band gap around the fermi level when it is supported on patterned hydrogen-terminated Si(001):1?×?1 surface. However, the band gap is reduced when a transverse electric field is applied, allowing the (3,3) CNT on the patterned hydrogen-terminated Si(001):1?×?1 to become metallic at a critical field strength. The tuning of electrical properties of the (3,3) CNT integrated with Si surface may have potential technological applications.     

Phase transition from asymmetric to symmetric dimer structure on the Si(001) surface at high temperature

The dimer configurations on the Si(001) surface at high temperatures have been investigated using the rocking curve of reflection high-energy electron diffraction. The Si(001) surface shows a displacive phase transition around 900 K, where a well-known asymmetric (tilted) dimer structure on the Si(001) at room temperature transforms to a symmetric dimer structure around 900 K. The metallic feature of the Si(001) surface above 900 K can be explained by the phase transition.     

Valence surface electronic states on Ge(001)

The optical, electrical, and chemical properties of semiconductor surfaces are largely determined by their electronic states close to the Fermi level (E{F}). We use scanning tunneling microscopy and density functional theory to clarify the fundamental nature of the ground state Ge(001) electronic structure near E{F}, and resolve previously contradictory photoemission and tunneling spectroscopy data. The highest energy occupied surface states were found to be exclusively back bond states, in contrast to the Si(001) surface, where dangling bond states also lie at the top of the valence band.     

Chemisorption of Fe on Au-passivated Si（001） surface

The chemisorption of one monolayer of Fe atoms on a Au-passivated Si(001) surface is studied by using the self-consistent tight-binding linear muffin-tin orbital method. The Fe adatom chemisorption on an ideal Si(001) surface is also considered for comparison. The chemisorption energy and layer projected density of states for a monolayer of Fe atoms on Au-passivated Si(001) surface are calculated and compared with that of the Fe atoms on an ideal Si(001) surface. The charge transfer is investigated. It is found that the most stable position is at the fourfold hollow site for the adsorbed Fe atoms, which might sit below the Au surface. Therefore there will be a Au－Fe mixed layer at the Fe/Au－Si(100) interface. It is found that the adsorbed Fe atoms cannot sit below the Si surface, indicating that a buffer layer of Au atoms may hinder the intermixing of Fe atoms and Si atoms at the Fe/Au－Si(001) interface effectively, which is in agreement with the experimental results.     

Order-disorder transition on Si(001): c(4 × 2) to (2 × 1)

A phase transition between c(4 × 2) and (2 × 1) structures on the clean Si(001) surface has been observed at about 200 K by low energy electron diffraction. From the temperature dependence of the width and intensity of the diffraction spots this transition is concluded to be a second order order-disorder transition. The transition proceeds by a single stage, which is in strong contrast with the case of Ge(001) for which a two-stage transition has been reported.     

Sb/Si(001)表面的半经验研究

用基于Chadi模型和格林函数方法的一种计算表面应力的半经验方法研究了Sb吸附在Si(001) 衬底上的性质.结果显示,Sb原子在Si(001)表面形成对称的dimer,其键长为0.293nm,表 面以下层的弛豫很小.Sb/Si(001)2×1表面沿着dimer方向的张应力为1.0eV/(1×1cell),而 沿垂直于dimer方向的压应力为-1.1eV/(1×1cell).Sb/Si(001)表面应力的主要贡献来自于 最上面三层表面. 关键词： 表面应力 异质生长 格林函数方法     

Atomic and electronic properties of tert-butanol on the Si(001)-(2×1) surface

The atomic and electronic properties of the adsorption of tert-butanol [(CH₃)₃OH] molecule on the Si(001)-(2×1) surface have been studied by using the ab-initio density functional theory (DFT) based on pseudopotential approach. We have found that tert-butanol bonded the Si(001) surface by oxygen atom, cleaving a O–H bond and producing a Si-H bond and tert-butoxy surface species. We have also investigated the influence of chemisorption of tert-butanol on the electronic structure of the clean Si(001)-(2×1) surface. Two occupied surface states situated entirely below the bulk valence band maximum have been identified, which means that the clean Si(001)-(2×1)surface was passivated by the chemisorption of tert-butanol. In order to explain the nature of the surface components we have also plotted the total and partial charge densities at the [`(K)]\bar{K} point of the surface Brillouin zone (SBZ).     

Structural and phase transformations during initial stages of copper condensation on Si(001)

Auger-electron spectroscopy, electron-energy loss spectroscopy, low-energy electron diffraction, and atomic-force microscopy are employed to investigate the growth mechanism, composition, structural and phase states, and morphology of Cu films (0.1–1 nm thick) deposited on a Si(001)-2 × 1 surface at a lower temperature of Cu evaporation (900°C) and room temperature of a substrate. The Cu film phase is shown to start growing on the Si(001)⁻² × 1 surface after three Cu monolayers (MLs) are condensed. It has been revealed that atoms of Cu and Si(001) are mixed, a Cu₂Si film phase is formed, and, thereafter, Cu₃Si islands arise at a larger coating thickness. Annealing of the first Cu ML leads to reconstruction of the Si(001)-1 × 1-Cu surface layer, thereby modifying the film growth mechanism. As a consequence, the Cu₂Si film phase arises when the thickness reaches two to four MLs, and bulk Cu₃Si silicide islands begin growing at five to ten MLs. When islands continue to grow, their height and density reach, respectively, 1.5 nm and 2 × 10¹¹ cm⁻² and the island area is 70% of the substrate surface at a thickness of ten MLs.