Deviations from exact epitaxial positions in heteroepitaxy

Epitaxy provides thin films in a perfect periodic structure. In heteroepitaxy the misfit may yield perfect pseudomorphic films or relaxed films, which may show the periodicities of the substrate and the film and their combinations. Then non-periodic defects like mosaics may appear, e.g., due to dislocations. Deviations from exact epitaxial positions in strictly periodic structures can be determined from diffraction intensities. For more complex surfaces, e.g., films with defects like mosaics or large superstructures or on substrates with steps such a strict determination is not possible. From the spot profile analysis of low energy electron diffraction (LEED) or X-ray data some structural information is available for these surfaces with defects. This new type of evaluation is demonstrated with spot profile analysis of LEED (SPA-LEED) for ultrathin Pb films on Si(1 1 1)7 × 7 surface, which grow even at 25 K epitaxially in a layer-by-layer growth mode. The analysis provides the first information on deviation from the exact epitaxial positions of the surface Pb atoms. A vertical shift of domains and an inclination between domains provides an explanation of the experimental results.     

Effect of CoSi2 buffer layer on structure and magnetic properties of Co films grown on Si（001） substrate

Buffer layer provides an opportunity to enhance the quality of ultrathin magnetic films.In this paper,Co films with different thickness of Co Si2buffer layers were grown on Si(001)substrates.In order to investigate morphology,structure,and magnetic properties of films,scanning tunneling microscope(STM),low energy electron diffraction(LEED),high resolution transmission electron microscopy(HRTEM),and surface magneto-optical Kerr effect(SMOKE)were used.The results show that the crystal quality and magnetic anisotropies of the Co films are strongly affected by the thickness of Co Si2buffer layers.Few Co Si2monolayers can prevent the interdiffusion of Si substrate and Co film and enhance the Co film quality.Furthermore,the in-plane magnetic anisotropy of Co film with optimal buffer layer shows four-fold symmetry and exhibits the two-jumps of magnetization reversal process,which is the typical phenomenon in cubic(001)films.     

Ultra-thin film growth of titanium dioxide on W(1 0 0)

We have employed low energy electron diffraction (LEED) and X-ray photoelectron spectroscopy to follow the epitaxial growth of thin films of TiO₂ on W(1 0 0). The films were grown both by metal vapour deposition of titanium onto the substrate in UHV with subsequent annealing in a low partial pressure of oxygen, and by metal vapour deposition in a low partial pressure of oxygen. LEED patterns showed the characteristic patterns of (1 1 0) oriented rutile. A systematic spot splitting was observed and attributed to a stepped surface. The calculated step height was found to be in good agreement with that expected for rutile TiO₂(1 1 0), 3.3 Å. Titanium core level shifts were used to identify oxidation states as a function of film thickness allowing the interpretation in terms of a slightly sub-stoichiometric interface layer in contact with the substrate. In combination with the LEED patterns, the film structure is therefore determined to be (1 1 0) oriented rutile with a comparable level of stoichiometry to UHV prepared bulk crystals. The ordered step structure indicates considerable structural complexity of the surface.     

Interface structures and rotational epitaxy of titanium on tungsten (110)

Interface structures of ultrathin Ti films grown on W(110) have been studied by low energy electron diffraction (LEED) and Auger electron spectroscopy (AES) in a wide range of annealing temperatures. The interface structures observed are interpreted to be due to site-coincidence growth (commensurate growth) and rotational epitaxy (incommensurate growth), respectively. The first monolayer of titanium is very strained with a large unit-cell expansion of 12.7% relative to that of Ti(0001). Deposition of additional Ti atoms destroys the strained structure, leading to rotational epitaxy: two Ti(0001) domains rotating mutually by 9.9 °. A thermally stable Ti bilayer exists at high annealing temperatures.     

Chiral surfaces and metal/ceramic heteroepitaxy in the Pt/SrTiO3(621) system

Low-energy electron diffraction (LEED), atomic force microscopy (AFM), and X-ray diffraction (XRD) have been used to investigate the structural and morphological character of a naturally chiral ceramic SrTiO₃(621) substrate and of Pt and Cu thin films deposited on its surface. AFM experiments showed that as-received chirally-oriented SrTiO₃(621) substrates display atomically smooth surface morphologies, while LEED patterns revealed that the surface structure has a net chirality. Pt(621) and Cu(621) thin films were grown heteroepitaxially on SrTiO₃(621) substrates, as confirmed by XRD. AFM showed that the film surfaces were atomically smooth and LEED illustrated that the Pt films exhibit surface chirality, and by implication that the atomically-flat chirally-oriented Cu films also have chiral surfaces. The characteristics of the observed LEED patterns, where splitting of diffraction spots is considered to arise from the kinked step features of naturally chiral fcc metal surfaces, are discussed with respect to existing models. These results indicate that the chiral SrTiO₃(621) ceramic surface drives the growth of single-enantiomer, chiral, metal (621) thin films.     

Crystallography and morphology of the early stages of the growth of CoCu(111) by LEED and STM

We report on a quantitative investigation of the structure and morphology of ultrathin films of Co deposited on Cu(111) by an in situ combination of real space (STM) and diffraction (LEED) techniques. The film grows initially as bilayer islands with strict fcc stacking. part of them are covered by Cu. The lateral distribution of Co- and Cu-terminated domains as well as of uncovered patches is both quantitatively determined by intensity analysis and visualized by STM images. Their simultaneous presence correlates nicely to known magnetic properties of ultrathin films, in particular with the observed magnetic anisotropy.     

Structure and electronic properties of ultrathin Co films on W(1 1 0)

The structure and electronic properties of ultrathin Co films on W(1 1 0) grown by molecular beam epitaxy in UHV were investigated by low energy electron diffraction (LEED) and scanning tunneling microscopy and spectroscopy (STM and STS). For coverages above 0.7 ML the pseudomorphic (ps) monolayer is transformed gradually into close-packed (cp-) monolayer areas, showing up as separated islands that increase in size with coverage until the cp-monolayer is complete. Two different structures of the cp-monolayer were observed by atomically resolved STM, both leading to a 8 × 1 superstructure in the LEED pattern. Higher coverages continue to grow in the Stransky–Krastanov growth mode forming simultaneously double layer islands and triple layer islands in fcc(1 1 1) and hcp(0 0 0 1) stacking. STS reveals tunneling spectra that differ considerably depending on the thickness and on the structure. Two different classes of triple layer islands can be distinguished by a resonant peak at +0.3 eV appearing in only one of the two classes. We attributed this behavior to a different stacking according to a fcc or hcp structure.     

The growth mode of aluminium on silver (111)

The geometric and electronic structures occuring during the growth of Al on a single crystal Ag(111) surface have been studied using a combination of low energy electron diffraction (LEED), Auger electron spectroscopy (AES), energy loss spectroscopy (ELS) and work function measurements. The Auger signal versus deposition time plots, which were used to monitor the growth mode, are shown to behave in an identical fashion to that expected for layer-by-layer (Frank-van der Merwe) growth. LEED was used to determine the lateral periodicity of thin Al films and shows that Al forms, at very small coverages, 2D islands which have the same structure as the Ag(111) substrate and which grow together to form the first monolayer. At substrate temperatures of 150 K a well defined (1 × 1) structure with the same orientation as the underlying Ag(111) can be seen up to at least 12 ML. After completion of the third monolayer the ELS spectrum approached that observed for bulk aluminium. At a coverage of 3 ML the work function decreases by 0.4 eV from the clean silver value.     

Strain analysis of epitaxial ultrathin films on Pt(111)

X-ray photoelectron diffraction (XPD) measurements have demonstrated that Ni ultrathin films on Pt(111) exhibit a single domain fcc stacking pseudomorphic to the substrate, with a consequent trigonal distortion of the Ni unit cell in order to accommodate the in-plane expansion of the Ni lattice parameter of about 11% with respect to its bulk value. We show that the amount of interlayer contraction and the strain energy resulting form the trigonal distortion are very well predicted by a strain analysis in the framework of simple linear elasticity theory. Strain analysis also allows to discuss in some detail the controversial case of Co growth on the same substrate. Finally, we discuss the dependence of the strain energy of the overlayer on the substrate crystal orientation and its effects on chemisorption experiments performed on heteroepitaxial monolayers (HML).     

Electronic structure of molecular beam epitaxy grown 1T'-MoTe_2 film and strain effect

Atomically thin transition metal dichalcogenide films with distorted trigonal(1T') phase have been predicted to be candidates for realizing quantum spin Hall effect. Growth of 1T' film and experimental investigation of its electronic structure are critical. Here we report the electronic structure of 1T'-MoTe_2 films grown by molecular beam epitaxy(MBE).Growth of the 1T'-MoTe_2 film depends critically on the substrate temperature, and successful growth of the film is indicated by streaky stripes in the reflection high energy electron diffraction(RHEED) and sharp diffraction spots in the low energy electron diffraction(LEED). Angle-resolved photoemission spectroscopy(ARPES) measurements reveal a metallic behavior in the as-grown film with an overlap between the conduction and valence bands. First principles calculation suggests that a suitable tensile strain along the a-axis direction is needed to induce a gap to make it an insulator. Our work not only reports the electronic structure of MBE grown 1T'-MoTe_2 films, but also provides insights for strain engineering to make it possible for quantum spin Hall effect.     

A new ultra‐high‐vacuum variable temperature and high‐magnetic‐field X‐ray magnetic circular dichroism facility at LNLS

X‐ray magnetic circular dichroism (XMCD) is one of the most powerful tools for investigating the magnetic properties of different types of materials that display ferromagnetic behavior. Compared with other magnetic‐sensitive techniques, XMCD has the advantage of being element specific and is capable of separating the spin and magnetic moment contributions associated with each element in the sample. In samples involving, for example, buried atoms, clusters on surfaces or at interfaces, ultrathin films, nanoparticles and nanostructures, three experimental conditions must be present to perform state‐of‐the‐art XMCD measurements: high magnetic fields, low temperatures and an ultra‐high‐vacuum environment. This paper describes a new apparatus that can be easily installed at different X‐ray and UV beamlines at the Brazilian Synchrotron Light Laboratory (LNLS). The apparatus combines the three characteristics described above and different methods to measure the absorption signal. It also permits in situ sample preparation and transfer to another chamber for measurement by conventional surface science techniques such as low‐energy electron diffraction (LEED), reflection high‐energy electron diffraction (RHEED), X‐ray photoelectron spectroscopy (XPS) and X‐ray photoelectron diffraction (XPD). Examples are given of XMCD measurements performed with this set‐up on different materials.     

GaN nucleation on (0 0 0 1)-sapphire via ion-induced nitridation of gallium

The growth of epitaxial GaN films on (0 0 0 1)-sapphire has been investigated using X-ray photoelectron spectroscopy (XPS) and low energy electron diffraction (LEED). In order to investigate the mechanism of the growth in detail, we have focused on the nitridation of pre-deposited Ga layers (droplets) using ion beam-assisted molecular beam epitaxy (IBA-MBE). Comparative analysis of XPS core-level spectra and LEED patterns reveals, that nitride films nucleate as epitaxial GaN islands. The wetting of the surface by GaN proceeds via reactive spreading of metallic Ga, supplied from the droplets. The discussed growth model confirms, that excess of metallic Ga is beneficial for GaN nucleation.     

Energy-dependent cancellation of diffraction spots due to surface roughening

The low-energy electron diffraction (LEED) pattern of the step-kinked Pt{531} surface at 200 K shows energy-dependent cancellation of diffraction spots over unusually large energy ranges, up to 100 eV. This cannot be reproduced theoretically when a flat surface geometry is assumed. A relatively simple model of roughening, however, involving 0.25 ML of vacancies and adatoms leads to very good agreement with the experiment. The cancellation of intensities within a very narrow range of adatom or vacancy coverages is caused by the interference of electrons emerging from different heights but similar local environments. This is a rare example where the energy dependence of integrated LEED spot intensities is dramatically affected by the long-range arrangement of atoms.     

Magnetization reversal of ultrathin Fe film grown on Si（111） using iron silicide template

Ultrathin Fe films were epitaxially grown on Si（lll） by using an ultrathin iron silicide film with p（2 × 2） surface reconstruction as a template. The surface structure and magnetic properties were investigated in situ by low energy electron diffraction （LEED）, scanning tunnelling microscopy （STM）, and surface magneto-optical effect （SMOKE）. Polar SMOKE hysteresis loops demonstrate that the Fe ultrathin films with thickness t 〈 6 ML （monolayers） exhibit perpen-dicular magnetic anisotropy. The characters of M-H loops with the external magnetic field at difference angles and the angular dependence of coercivity suggest that the domain-wall pinning plays a dominant role in the magnetization reversal process.[第一段]     

Me-PTCDI thin film deposition on InSb(1 1 1)A

The evolution of N,N′-dimethylperylene-3,4,9,10-dicarboxyimide (Me-PTCDI) thin films formed by vapour deposition on InSb(1 1 1)A substrates has been studied by X-ray photoelectron spectroscopy (XPS), high-resolution electron energy loss spectroscopy (HREELS) and low energy electron diffraction (LEED). XPS studies of the Me-PTCDI covered surface indicate that no significant interaction occurs at sub-monolayer coverage when compared to multilayer Me-PTCDI films. HREELS studies suggest only a weak interaction as evidenced by very small changes in the frequencies of several molecular vibrational modes. LEED patterns show the Me-PTCDI overlayer adopts a structure commensurate with the underlying InSb(1 1 1)A substrate surface and that can be rationalised by van der Waals intermolecular energy calculations for the Me-PTCDI unit cell. The results are consistent with a weak interaction at the Me-PTCDI/InSb interface, the formation of the commensurate structure being sufficient to overcome the small energetic penalty associated with deviation from the calculated intermolecular interaction energy minimum.     

Moiré pattern in LEED obtained by van der Waals epitaxy of lattice mismatched WS2/MoTe2(0001) heterointerfaces

Thin films of WS₂ have been grown by van der Waals epitaxy (vdWE) on the basal planes of 2H-MoTe₂(0001). Despite a lateral mismatch of 10.3%, epitaxial growth is achieved by metal organic vdWE (MOvdWE). In low energy electron diffraction (LEED) measurements a Moiré-like superstructure is observed originating from and correlated to the lateral mismatch between film and substrate. I–V LEED investigations in the course of sequential film growth reveal an undulation of the lattice at the interfaces as the origin of the Moiré-like structure rather than simple multiple scattering between overlayer and substrate.     

Structure of V thin films on Al(100) using XPD,LEED, and LEIS

We have used X-ray photoelectron diffraction (XPD), low energy electron diffraction (LEED), and low energy ion scattering (LEIS) to determine the atomic structure of V thin films grown on the Al(100) single crystal surface. For V film thicknesses ranging from 0.75 ML–7 ML, the LEED patterns show no significant changes from the p(1 × 1) symmetry of a clean Al(100) surface, other than becoming more diffuse for higher V coverage. XPD and LEIS spectra indicate that during the initial deposition (1–3 ML) V atoms diffuse into the Al lattice, and tend to accumulate at the surface during subsequent deposition. Strain associated with the lattice mismatch for V and Al is likely relieved by the formation of a surface alloy during the first few ML's of V deposition. For 7 ML V coverage, XPD and LEED showed that an ordered V structure is stabilized on the Al(100) surface. Due to the close resemblance of the V and Al XPD polar scans, we conclude that V and Al are occupying similar lattice sites in tetragonally distorted bcc lattice, although the specific lattice location of the V and Al atoms is not clear.     

Correlation of electron self-energy with geometric structure in low-energy electron diffraction

In low-energy electron diffraction (LEED) studies of surface geometries where the energy dependence of the intensities is analyzed, the in-plane lattice parameter of the surface is usually set to a value determined by x-ray diffraction for the bulk crystal. In cases where it is not known, for instance in films that are incommensurate with the substrate, it is desirable to fit the in-plane lattice parameters in the same analysis as the perpendicular interlayer spacings. We show that this is not possible in a conventional LEED I(E) analysis because the inner potential, which is typically treated as an adjustable parameter, is correlated with the geometrical structure. Therefore, without having prior knowledge of the inner potential, it is not possible to determine the complete surface structure simply from LEED I(E) spectra, and the in-plane lattice parameter must be determined independently before the I(E) analysis is performed. This can be accomplished by establishing a more precise experimental geometry. Further, it is shown that the convention of omitting the energy dependency of the real part of the inner potential means geometrical LEED results cannot be trusted beyond a precision of approximately 0.01 ?.     

LEED studies on stepped W surfaces

Steps on single crystal surfaces have been shown to cause changes of various physical properties and to influence the behaviour towards chemical reactions. A proper knowledge of the step structure is required for the understanding of these phenomena. The following investigation concentrates on a detailed evaluation of the LEED patterns of various stepped tungsten surfaces. A formula is given for determining the terrace width of ordered step arrays from any diffraction order. Step height, step orientation, terrace width and the sample orientation have been deduced from the LEED patterns and the experimental errors involved are being discussed. The step height can be determined within 1% and the terrace width within 1 to 3% depending on the step density. It is concluded that the determination of the sample orientation as obtained from the LEED pattern is at least as precise as by using the Laue X-ray back reflection technique.     

Formation of a passive layer in surface oxidation of Gd: A leed and AES study

The surface oxidation of epitaxial and polycrystalline Gd samples grown in ultrahigh vacuum on W(110) substrates has been investigated using Auger-electron spectroscopy (AES) and low energy electron diffraction (LEED). The surface crystallography of clean epitaxial films monitored by LEED is hcp(0001) and remains unchanged even after 300 L oxygen exposure at room temperature. The LEED pattern of bulk Gd₂O₃ in Mn₂O₃ structure is observed only when oxygen is exposed at an elevated substrate temperature of about 500°C. AES clearly reveals various stages of oxidation as a function of the oxygen exposure for epitaxial as well as polycrystalline films. It is found that the oxidation does not proceed beyond one monolayer of the Gd surface.