Relativistic electronic structure calculations on endohedral Gd@C60, La@C60, Gd@C74, and La@C74

We have investigated the adsorption of Ba on the Si(111) surface at elevated temperatures by using high-resolution electron-energy-loss spectroscopy, low-energy-electron diffraction, and photoelectron spectroscopy with synchrotron photons. We found two new ordered phases 2×1a and 2×1bwith increasing Ba coverage in addition to other ordered phases reported earlier. All the ordered surfaces were found to remain semiconducting with a hybridization band gap of ∼1.1 eV almost independent of Ba coverage. We discuss evidence for the evolution of a Ba s-s hybridization band for Ba coverage beyond 0.5 monolayers and propose structural models for the three ordered phases, which are quite consistent with our experimental data. Received: 16 May 2000 / Accepted: 17 May 2000 / Published online: 16 August 2000     

3D DuMond diagrams of multi-crystal Bragg-case synchrotron topography. II. Curved sample

The dimensional features of multi-crystal synchrotron X-ray topographs are explained by 3D DuMond diagrams for a flat double-crystal monochromator and a curved sample. Symmetric Bragg-case reflections are assumed for all crystals. σ–σ and σ–π geometries are considered, where the diffraction plane of the sample is parallel and perpendicular, respectively, to the vertical diffraction plane of the monochromator (σ polarization). It is shown that the shape of the sample image is closely connected to the shape of the volume shared by the diffraction domains of monochromator and sample in the 3D DuMond diagram. In particular, for the σ–π set-up, the image shape depends on the curvature value and sign. An experiment is reported for this latter crystal geometry to determine lattice mismatch, its lateral homogeneity and curvature value and sign in a sample made of epilayer and substrate. Received: 31 July 2000 / Accepted: 25 January 2001 / Published online: 26 April 2001     

3D DuMond diagrams of multi-crystal Bragg-case synchrotron topography. I. Flat sample

The 3D representation of the DuMond diagram is used to explain the dimensional features of X-ray topographs obtained by multi-crystal configuration with a synchrotron beam. Symmetric Bragg-case reflections are considered for a flat double-crystal monochromator and a flat sample. Two ways of sample alignment are taken into account. They are referred to as σ–σ and σ–π geometries, where the diffraction plane of the sample is parallel and perpendicular, respectively, to the vertical diffraction plane of the monochromator (σ polarization). It is shown that the shape of the sample image is closely connected to the shape the diffraction domain common to monochromator and sample assumes in the 3D DuMond diagram. An experiment is reported for the less commonly used σ–π topography, showing how the lattice mismatch and its lateral homogeneity are determined in samples made by epilayer and substrate. Received: 31 July 2000 / Accepted: 25 January 2001 / Published online: 3 May 2001     

Droplet velocity and acceleration measurements in dense sprays by laser flow tagging

The feasibility of liquid-phase velocity measurements in dense sprays by 2D laser-based flow tagging is demonstrated. Velocity measurements in dense sprays are difficult with conventional techniques because of the high number densities of droplets, the optical thickness of the medium, and multiple light-scattering effects. The present flow-tagging technique is based on phosphorescent tracer molecules, which are excited by a grid of pulsed ‘write’ laser beams. The motion of the tagged droplet groups can be observed by a CCD camera in this way. In addition, multiple consecutive velocity measurements are performed by ‘droplet-group tracking’. This yields the acceleration along the trajectory of individual groups of droplets in unsteady sprays. Received: 5 June 2000 / Revised version: 28 July 2000 / Published online: 6 September 2000     

Structural and optical properties of nanophase zinc oxide

Nanophase zinc oxide samples were synthesized by a two-step solid-state reaction method. The phase structure and microstructure were investigated by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The vibrational Raman spectra were compared with those from the bulk and their grain size dependence was also examined. Their photoelectric behavior was studied by X-ray photoelectron spectroscopy (XPS). The peaks at 1044.5 and 1021.4 eV were recorded as corresponding to the respective binding energies of Zn 2p_1/2 and Zn 2p_3/2, and the photoelectron spectrum of O 1s in the as-prepared powder was located at 531.2 eV. A strong visible emission centered at 580 nm was clearly observed in the nanosized zinc oxide at room temperature. Photoluminescence (PL) spectra were investigated as a function of grain size after different heat treatments. The origin of the luminescence is attributed to the recombination of electrons in singly occupied oxygen vacancies with photoexcited holes in the valence band. Received: 30 June 2001 / Accepted: 20 February 2002 / Published online: 3 June 2002 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: mszhang@nju.edu.cn     

Photoelectron spectroscopic characterization of titanium-containing amorphous hydrogenated silicon–carbon films (aSi1-xCx:H/Ti)

Titanium-containing amorphous hydrogenated silicon–carbon films (aSi_1-xC_x:H/Ti) have been deposited by reactive magnetron cosputtering. Core-level photoelectron spectroscopy (XPS) and valence-band photoelectron spectroscopy (UPS) have served as means for the characterization of these films. The spectroscopic data are interpreted by a structural model on the basis of a nanocomposite containing clusters of a Ti-C-Si alloy being embedded in an amorphous hydrogenated silicon–carbon matrix (aSi_1-xC_x:H). The Ti-C-Si compound is of metallic character and most likely a substitutional solid solution. This novel nanocomposite material is a promising candidate for applications, especially as optical selective absorber coating for solar collectors. Received: 10 July 2000 / Accepted: 15 September 2000 / Published online: 21 March 2001     

Photoelectron diffraction: from phenomenological demonstration to practical tool

The potential of photoelectron diffraction—exploiting the coherent interference of directly-emitted and elastically scattered components of the photoelectron wavefield emitted from a core level of a surface atom to obtain structural information—was first appreciated in the 1970s. The first demonstrations of the effect were published towards the end of that decade, but the method has now entered the mainstream armoury of surface structure determination. This short review has two objectives: First, to outline the way that the idea emerged and the way this evolved in my own collaboration with Neville Smith and his colleagues at Bell Labs in the early years: Second, to provide some insight into the current state-of-the art in application of (scanned-energy mode) photoelectron diffraction to address two key issue in quantitative surface structure determination, namely, complexity and precision. In this regard a particularly powerful aspect of photoelectron diffraction is its elemental and chemical-state specificity.     

Clusters on surfaces: high-resolution spectroscopy at low temperatures

With controlled growth in nanometer-sized pits we produced silver and gold clusters on a graphite surface. We give a summary of the preparation method and discuss the scanning tunneling imaging and the crystalline orientation of the clusters. The electronic structure of the clusters was studied by an in-situ combination of ultraviolet photoelectron spectroscopy (UPS) and scanning tunneling spectroscopy (STS). For both techniques we obtained an energy resolution in the range of 10 meV employing low sample temperatures. Dynamic final-state effects together with averaging over a cluster-size distribution result in characteristic spectral shapes in UPS, which can be understood referring to STS data taken on individual clusters. Finally, directions for future experiments are pointed out. Received: 13 April 2000 / Accepted: 6 November 2000 / Published online: 9 February 2001     

The structure of methoxy species on Cu(110): A combined photoelectron diffraction and density functional theory determination

The local structure of the methoxy species on Cu(110) has been investigated experimentally using chemical-state specific O 1s scanned-energy mode photoelectron diffraction (PhD), and also by density functional theory (DFT) calculations. The PhD data show a clear preference for adsorption with the O bonding atoms in short-bridge sites, though the best fit of multiple-scattering simulations to the experimental data is achieved with two slightly different short-bridge geometries. The DFT calculations also show that not only are the short-bridge sites energetically favoured in isolation, but that coordination to pairs of Cu adatoms has a similar energy. A structure consistent with both the PhD data and the DFT calculations is proposed for the previously-observed (5 × 2)pg ordered phase, based on methoxy species in short-bridge sites on pairs of Cu adatoms and on the underlying surface. Simulated scanning tunnelling microscopy images agree well with those observed experimentally, while the model is also shown to be consistent with the qualitative behaviour seen in early X-ray photoelectron diffraction (XPD) forward-scattering experiments.     

Metal-induced solid-phase crystallization of hydrogenated amorphous silicon: dependence on metal type and annealing temperature

We report on metal (Cr, Ni, or Pd)-induced solid-phase crystallization (MISPC) of plasma-enhanced chemical-vapor-deposited hydrogenated amorphous silicon at annealing temperatures ≤600 °C. MISPC is found to significantly reduce the thermal budget of crystallization at annealing temperatures as low as ∼400 °C. The lowest achievable annealing temperature is found to depend on the metal type. The metal type is also found to influence grain size and the conductivity of the polycrystalline silicon. Received: 21 June 1999 / Accepted: 20 October 1999 / Published online: 23 February 2000     

Structural,optical and electrical properties of sulfur-incorporated amorphous carbon films

Amorphous carbon–sulfur (a-C:S) composite films were prepared by vapor phase pyrolysis technique. The structural changes in the a-C:S films were investigated by electron microscopy. A powder X-ray diffraction (XRD) study depicts the two-phase nature of a sulfur-incorporated a-C system. The optical bandgap energy shows a decreasing trend with an increase in the sulfur content and preparation temperature. This infers a sulfur incorporation and pyrolysis temperature induced reduction in structural disorder or increase in sp ² or π-sites. The presence of sulfur (S 2p) in the a-C:S sample is analyzed by the X-ray photoelectron spectroscopy (XPS). The sp ³/sp ² hybridization ratio is determined by using the XPS C 1s peak fitting, and the results confirm an increase in sp ² hybrids with sulfur addition to a-C. The electrical resistivity variation in the films depends on both the sulfur concentration and the pyrolysis temperature.     

Buried interfaces studied by photoelectron diffraction

Angle- and energy-scanned photoelectron diffraction data can be used to investigate structures below surfaces. The modulations in photoelectron intensity result from diffraction of the emitted electron wave at neighbor atoms. In the past, scanned-energy photoelectron diffraction had been mainly used to determine the adsorption site of molecules at surfaces. Recent data show, however, that the technique can also be employed to obtain information about the upper substrate layer(s). At low kinetic energies, backward scattering is strong and in scanned-angle photoelectron diffraction the recorded patterns result from backward- and multiple-scattering effects. For a structural analysis, the intensity modulations have to be compared with the results for simulations performed for model clusters. As an example, recent angle-scanned photoelectron diffraction patterns recorded for the technologically important silicon oxide/silicon interface were compared with simulations. At the Si(001) surface orientation, the interface is extended over a few layers, whereas at the Si(111) surface orientation the transition is rather abrupt and occurs within one or two layers. Received: 9 September 2002 / Accepted: 2 October 2002 / Published online: 5 February 2003 RID="*" ID="*"Corresponding author. Fax: +49-231/755-3657, E-mail: carsten.westphal@physik.uni-dortmund.de     

Molar volume and compactness versus mean coordination number in GeSeFe glasses: observation of a threshold behavior

Molar volumes, V, and compactness values, α, of 34 glassy compositions of the GeSeFe system have been obtained using their measured densities. The property–composition dependences are examined in light of the models proposed for the structure of these network glasses. Received: 28 August 2000 / Accepted: 9 January 2001 / Published online: 23 March 2001     

Photo-ionization efficiency curves of alkali nanoclusters in a beam and determination of metal work functions

We produced free beams of cold nanometer-sized particles of lithium, sodium and potassium and measured the three corresponding photo-ionization yield curves. Quadratic (Fowler) plots, originally developed for bulk surfaces, were found to provide a good fit to the threshold shape and were used to obtain the particle ionization potentials. The latter match precisely the bulk work functions cited in the literature, suggesting that photo-ionization of free nanoclusters may form a useful complement to traditional photoelectron studies of surfaces. Within 0.25–1 eV above the threshold, the ionization efficiency begins to drop. This effect, which has parallels in bulk-surface and small-cluster photoemission, is presently not well understood but may be related to an interplay between electron emission and collective surface plasma excitations. Received: 21 June 2001 / Revised version: 7 July 2001 / Published online: 10 October 2001     

Evidence for the strain critical point in high Tc superconductors

We report experimental evidence for the phase diagram of doped cuprate superconductors as a function of the micro-strain of the planar Cu-O bond length, measured by Cu K-edge EXAFS, and hole doping . The local lattice distortions are measured by EXAFS and the charge ordering is measured by synchrotron radiation diffuse X-ray diffraction. This phase diagram shows a QCP at P() where for charge-orbital-spin stripes and free carriers co-exist. The superconducting phase occurs in the region of critical fluctuations around this QCP. The function of two variables shows its maximum at the strain QCP. The critical fluctuations near this strain QCP give the self-organization of a metallic superlattice of quantum wires “superstripes" that favors the amplification of the critical temperature. Received 25 September 2000     

CdTe epilayers for uses in optical waveguides

CdTe epilayers have been grown by vapor phase epitaxy (VPE) on glass, MgO, sapphire, LiNbO₃ and mica substrates. Scanning electron microscopy (SEM) and X-ray diffraction (XRD) studies show the good structural quality of the epilayers. In these epilayers, a few optical modes were excited with a 1.33-μm laser. The measured propagation losses were in the range between 5 dB/cm and less than 0.5 dB/cm. From dark-mode m-lines, the epilayer thickness was found to be in the 1–3 μm range, in good accord with that obtained by SEM measurements. The refractive index obtained from the fitting is also in good accord with that of bulk CdTe. Received: 7 October 1999 / Accepted: 13 March 2000 / Published online: 5 July 2000     

Break-up of neutron-halo nuclei by diffraction dissociation and shakeoff

The interplay of diffraction dissociation and nuclear shakeoff is considered in a schematic but still realistic model for the case of the break-up of halo nuclei on light targets. We demonstrate that the shakeoff effect, arising from the momentum imparted by the core diffraction, is small but still identifiable in the experimental data for the dissociation of the one- and two-neutron halo nuclei ¹¹Be and ¹¹Li. Received: 29 October 1999 / Revised version: 15 January 2000     

Prompt light particle emission in the 36Ar + 58Ni reaction at 95 MeV/nucleon

The prompt component at intermediate velocity of light charged particles is investigated. An improved coalescence model coupled to the intra-nuclear cascade code ISABEL is used to obtain light complex particle energy spectra and multiplicities as a function of impact parameter. The results are compared with experimental data from the ³⁶Ar + ⁵⁸Ni experiment at 95 MeV/nucleon, performed with the INDRA 4π detection system. The calculated prompt component is found to rather well reproduce proton spectra. For complex light charged particles the calculated components well populate the high energy part of spectra. Prompt emission can therefore explain the large transverse energies experimentally observed at mid-rapidity. Received: 27 July 2000 / Accepted: 20 November 2000     

Parallel excitation pathways in ultrafast interferometric pump-probe correlation measurements of hot-electron lifetimes in metals

Hot electron (E-E_Fermi=0.75 to 1.55 eV) lifetimes for cesiated Cu(100) and Cu(111) surfaces are measured via interferometric time-resolved two-photon photoemission with a 19-fs intensity FWHM mode locked Ti:sapphire laser at 1.55 eV. The data are analyzed using the optical Bloch equations and a laser pulse characterized in situ via surface second-harmonic generation interferometric autocorrelation. It is found that the retrieved hot-electron lifetimes are unphysically fast, and have a strong dependence on the temperature of the sample and the polarization of the laser. A simple explanation for the data is that the measured signal consists of contributions from transitions through both virtual and real intermediate states. Received: 26 July 2000 / Accepted: 8 September 2000 / Published online: 12 October 2000     

Synthesis and properties of In2(Se1-xTex)3 thin films: a new semiconductor compound

In₂(Se_1-xTe_x)₃ polycrystalline films were prepared by a dual-source thermal evaporation technique. The depositions onto glass and SnO₂-coated glass substrates were carried out in a vacuum chamber and followed by an annealing in neutral ambient (Ar or N₂). The structural, morphological and compositional studies of the films were made by X-ray diffraction, energy-dispersive X-ray analysis, X-ray photoelectron spectroscopy, scanning electron microscopy, Raman scattering and optical transmission. Optimum conditions are investigated for the formation of the ternary compound In₂(Se_1-xTe_x)₃ in order to tune the band gap by changing the Te concentration. The film properties as a function of Te amount are discussed. It is shown that single-phase, textured and homogeneous layers of In₂(Se_1-xTe_x)₃ can be grown with x≤0.2 at optimal deposition and heat treatment conditions. For x≅0.17 these films showed an energy band gap of about 1.45 eV and an electrical conductivity at room temperature six orders of magnitude higher than that of the binary γ-In₂Se₃ thin films. Received: 9 July 1999 / Accepted: 25 November 1999 / Published online: 13 July 2000