M. Degawa

Step bunching, step wandering and faceting: self-organization at Si surfaces

Step bunching, in-phase step wandering and faceting are new morphological evolutions from smooth vicinal surfaces. They are formed by giving changes of externally controlled parameters on surfaces. Two cases on Si surfaces are presented in detail. One is caused by unidirectional drift forces on adatoms on the surfaces, i.e., surface electromigration due to direct current specimen heating. Newly formed step instabilities are due to a change of a kinetic parameter on the surface. The other case is caused by adsorption of foreign metal atoms on the Si surfaces. In this case step instabilities are due to changes of thermodynamic parameters on the surface. Step bunching, in-phase step wandering and faceting processes in two cases are interesting dynamics of self-organization at surfaces and can be useful for microfabrication of surfaces. Recent results of these dynamic processes on vicinal surfaces of Si(1 1 1) and (0 0 1) surfaces and high index Si surfaces studied by real space and reciprocal space observation methods mainly done by our group are reviewed.

Direct Current Heating Induced Giant Step Bunching and Wandering on Si(111) and (001) Vicinal Surfaces

Direct current (DC) heating induced giant step bunching and wandering on Si(111) and (001) vicinal surfaces were newly found. The step bunching and wandering are so large that they can easily be studied by optical microscopy. Temperature dependence of the DC heating effects and the dependence of such effects on the crystallographic direction of the current were studied.

Direct-current-induced drift direction of silicon adatoms on Si(111)-(1×1) surfaces

Abstract The direction of the drift of adatoms induced by direct-current (DC) heating of Si(111)-(1×1) surfaces was studied from shape changes of a rectangular groove that was made by a focused ion beam (FIB) apparatus. It was found that the drift direction is to the current direction irrespective of the temperatures of the three ranges where DC-induced step-bunching behavior reverses twice. The result clearly shows that reversals of the current-induced step bunching are not due to reversals of the effective charge on silicon adatoms, but due to changes in the mechanism of step bunching.

Correlation time for step structural fluctuations

Time-dependent scanning tunneling microscopy has been used to evaluate step fluctuations as a function of temperature (300-450 K) on Ag(111) films grown on mica. The temporal correlation function scales as a power law in time t1/n with measured values of 1/n varying over a range of 0.19± 0.04 to 0.29±0.04 with no correlation on temperature. The average value of 1/n=0.24±0.01 is consistent with step-edge diffusion limited fluctuations (n=z=4, conserved noise). The magnitude of the time correlation function and the width of the fluctuations both scale with temperature with the same apparent activation energy of E eff =0.21±0.02 eV, indicating that the correlation time is at most weakly temperature dependent. Direct analysis of the autocorrelation function confirms that the correlation time is at most weakly temperature dependent, and thus the apparent correlation length is strongly temperature dependent. This behavior can be reproduced by assuming that the apparent correlation length is governed by the longest wavelength of step fluctuations that can be sampled in the measurement time interval. Evaluation of the correlation time for previous measurements for Al/Si(111) (z=2) yields the same conclusion about measurement time interval. In both cases the ratio of the measurement time to the effective correlation time is on the order of 10.

New Phase Diagram of Step Instabilities on Si(111) Vicinal Surfaces Induced by DC Annealing

On Si(111) vicinal surfaces, step bunching is observed when the sample is annealed with a direct current (DC). It is also known that the DC direction that induces step bunching changes three times ...

DC-HEATING-INDUCED ANTIBAND FORMATION AND SUBSEQUENT STEP WANDERING ON Si(111) STUDIED BY IN-SITU REM

Direct current fed through a Si crystal with (111) vicinal surfaces induces step bunching and wandering which depend on the temperature and the current direction. In the present report in-situ reflection electron microscope studies of antiband formation and the growth of step wandering are presented together with supplemental observations by scanning electron microscopy and optical microscopy. Observations were for the temperature range (about 1000–1180°C) where the step-down current induces step wandering and the step-up current induces step bunching and antiband formation and subsequent step wandering. An important role of antiband formation for step wandering in the step-up current regions is presented.

Temperature dependence of period of step wandering formed on Si(111) vicinal surfaces by DC heating

Wandering of an array of steps in phase on Si(111) vicinal surfaces (5° off toward the [11] direction) formed by DC heating at temperatures 1000<T<1180 °C was studied. Periods of the step wandering formed on step-down current regions depended on the temperature and had a maximum at around 1100 °C. This also supports the view that the wandering is due to the DC heating effect. The periods were also measured for the step wandering of anti-bands on terraces between step bands formed by DC heating with a step-up current and we found that the periods were appreciably smaller than that in the step-down current regions.Abstract:We investigate polaron formation in a many-electron system in the presence of a local repulsion sufficiently strong to prevent local-bipolaron formation. Specifically, we consider a Hubbard-Holstein model of interacting electrons coupled to dispersionless phonons of frequency . Numerically solving the model in a small one-dimensional cluster, we find that in the nearly adiabatic case , the necessary and sufficient condition for the polaronic regime to occur is that the energy gain in the atomic (i.e., extremely localized) regime overcomes the energy of the purely electronic system . In the antiadiabatic case, , polaron formation is instead driven by the condition of a large ionic displacement (g being the electron-phonon coupling). Dynamical properties of the model in the weak and moderately strong coupling regimes are also analyzed.

Time evolution of DC heating-induced in-phase step wandering on Si(111) vicinal surfaces

The time evolution of in-phase step wandering (IPSW) on Si(111) vicinal surfaces induced by direct current heating and its off-angle dependence were studied. The substrate temperature of 1100°C was chosen at which a wavelength of IPSW pattern is the maximum. The wavelength keeps nearly constant at approximately 7 μm as a function of annealing time and does not depend on off-angle. The amplitude of wandering steps in the IPSW pattern increases with annealing time and approaches its saturation value after 24 h, irrespective of off-angle. The saturation value depends on off-angle and decreases with increasing off-angle or decreasing mean step-step distance. This suggests that the amplitude of wandering steps is affected by step-step interaction.

Kinetic Parameters of Pb Obtained from Crystallite Evolutions

Issues in modeling the evolution of supported crystallites are addressed by fitting scanning tunneling microscopy (STM) measurements of the evolution of Pb crystallites using the formalism of the continuum step model. Initial and final states used in the calculations are the least-stable metastable states for a cylindrically symmetrical crystallite with step–step repulsions varying as the inverse separation squared. The step–step interaction strength is determined from fits to the final shape. The kinetic parameters (terrace diffusion and step detachment rate) are determined by fits to the rate of evolution of individual layers of the crystallite. Using the obtained experimental values, a numerical simulation with a fixed step chemical potential for the boundary condition is performed. The results greatly overestimate the critical slowing down as the crystallite approaches the final state.

Correlations in nanoscale step fluctuations: Comparison of simulation and experiments

We have recently argued that manganites do not possess stripes of charge order, implying that the electron-lattice coupling is weak [Loudon et al., Phys. Rev. Lett. 94, 097202 (2005)]. Here we independently argue the same conclusion based on transmission electron microscopy measurements of a nanopatterned epitaxial film of La{sub 0.5}Ca{sub 0.5}MnO{sub 3}. In strain relaxed regions, the superlattice period is modified by 2% to 3% with respect to the parent lattice, suggesting that the two are not strongly tied.Minimalist theories of complex systems are broadly of two kinds: mean field and axiomatic. So far, all theories of complex properties absent from simple systems and intrinsic to glasses are axiomatic. Stretched Exponential Relaxation (SER) is the prototypical complex temporal property of glasses, discovered by Kohlrausch 150 years ago, and now observed almost universally in microscopically homogeneous, complex nonequilibrium materials, including luminescent electronic Coulomb glasses. A critical comparison of alternative axiomatic theories with both numerical simulations and experiments strongly favors channeled dynamical trap models over static percolative or energy landscape models. The topics discussed cover those reported since the authors review article in 1996, with an emphasis on parallels between channel bifurcation in electronic and molecular relaxation.The local atomic structure of the Ag induced Si(111)-({radical}(3)x{radical}(3)) surface has been investigated using photoelectron diffraction (PED) at 10 and 300 K. Two surface components, whose intensities varied by changing the photon energy as a consequence of diffraction effects, were observed in the Si 2p core-level spectra at both temperatures. The good agreement between the experimental PED patterns of the Si 2p surface components and the simulated PED patterns indicates that the atomic structure of this surface follows the inequivalent triangle model. Further, since the PED patterns obtained at 10 and 300 K resemble each other closely, we conclude that the local atomic structure of the Ag/Si(111)-({radical}(3)x{radical}(3)) surface is the same at the two temperatures, and thus that the origin of the transition reported in the literature is an order-disorder transition.Neutron diffraction was used to determine the crystal structure and magnetic ordering pattern of a La{sub 2}CuO{sub 4} single crystal, with and without applied magnetic field. A previously unreported, subtle monoclinic distortion of the crystal structure away from the orthorhombic space group Bmab was detected. The distortion is also present in lightly Sr-doped crystals. A refinement of the crystal structure shows that the deviation from orthorhombic symmetry is predominantly determined to drive a continuous reorientation of the copper spins from the orthorhombic b axis to the c axis, directly confirming predictions based on prior magnetoresistance and Raman scattering experiments. A spin-flop transition induced by a c-axis oriented field previously reported for nonstoichiometric La{sub 2}CuO{sub 4} is also observed, but the transition field (11.5 T) is significantly larger than that in the previous work.Positron annihilation spectroscopy was applied to study relaxed P-doped n-type and undoped Si{sub 1-x}Ge{sub x} layers with x up to 0.30. The as-grown SiGe layers were found to be defect free and annihilation parameters in a random SiGe alloy could be represented as superpositions of annihilations in bulk Si and Ge. A 2 MeV proton irradiation with a 1.6x10{sup 15} cm{sup -2} fluence was used to produce saturated positron trapping in monovacancy related defects in the n-type layers. The defects were identified as V-P pairs, the E center. The distribution of Si and Ge atoms surrounding the E center was the same as in the host lattice. The process leading to the formation of V-P pairs therefore does not seem to have a significant preference for either Si or Ge atoms. In undoped Si{sub 1-x}Ge{sub x} we find that a similar irradiation produces a low concentration of divacancies or larger vacancy defects and found no evidence of monovacancies surrounded by several Ge atoms.Structural properties of the spin chain and ladder compound Sr{sub 14}Cu{sub 24}O{sub 41} have been studied using high energy x-ray diffraction. Strong incommensurate modulation reflections are observed due to the lattice mismatch of the chain and ladder structure, respectively. While modulation reflections of low orders display only a weak temperature dependence, higher orders dramatically increase in intensity when cooling the sample to 10 K. All observed modulation reflections are indexed within a super space group symmetry and no structural phase transition could be identified between 10 K and room temperature. We argue that these modulation reflections are not caused by a fivefold periodicity of the chain lattice, as claimed by Fukuda et al., Phys. Rev. B 66, 012104 (2002), but that holes localize in the potential given by the lattice modulation, which in turn gives rise to a further deformation of the lattice.We report neutron diffraction experiments on the light-induced metastable state SI in single crystals of Na{sub 2}[Fe(CN){sub 5}NO]{center_dot}2D{sub 2}O. It is shown that the metastable state SI corresponds to a linkage isomer of the NO group, the so-called isonitrosyl configuration where the NO ligand is oxygen bound to the central iron atom.The impact of group-III vacancy diffusion, generated during dielectric cap induced intermixing, on the energy state transition and the inhomogeneity reduction in the InGaAs/GaAs quantum-dot structure is investigated. We use a three-dimensional quantum-dot diffusion model and photoluminescence data to determine the thermal and the interdiffusion properties of the quantum dot. The band gap energy variation related to the dot uniformity is found to be dominantly affected by the height fluctuation. A group-III vacancies migration energy H{sub m} for InGaAs quantum dots of 1.7 eV was deduced. This result is similar to the value obtained from the bulk and GaAs/AlGaAs quantum-well materials confirming the role of SiO{sub 2} capping enhanced group-III vacancy induced interdiffusion in the InGaAs quantum dots.We report vibrating wire viscometer experiments in the concentrated and dilute phase of saturated {sup 3}He-{sup 4}He mixtures showing that the slip length may become orders of magnitude larger than the mean free path due to specular scattering of the {sup 3}He quasiparticles with a {sup 4}He coating adsorbed at the surface of the wire. Since the liquid does not almost stick to the surface, the boundary conditions for fluid flow are unusual and not accounted for by the current theory for slip [H. Hoejgaard Jensen et al., J. Low Temp. Phys. 41, 473 (1980)]. The experimental results are in excellent agreement with a recent theory for slip [R. Bowley and J. Owers-Bradley, J. Low Temp. Phys. 136, 15 (2004)] which accounts for the effect of the cylindrical geometry and for velocity slip in directions normal as well as tangential to the surface of the wire. We find that our viscosity measurements in the dilute phase resulting from the data analysis based on the recent slip theory are in better agreement with the Fermi liquid theory than previous experimental results.Magnetization measurements prove that the magnetic properties of large-angle ({theta}>30 deg. ) bismuth bicrystals with a crystallite interface (CI) of twisting types essentially differ from well-known results on single-crystalline specimens. Two superconducting phases with T{sub c}{approx}8.4 K and {approx}4.3 K were observed at the CI of bicrystals while ordinary rhombohedral Bi is not a superconductor. We conclude that these phases have to do with the central part and the adjacent layers of the CI of bicrystals.The local structure around Ag ions in silver borate glasses g-Ag{sub 2}O{center_dot}nB{sub 2}O{sub 3} (n=2,4) was studied by x-ray absorption spectroscopy at the Ag K edge for temperatures from 77 to 450 K. Extended x-ray absorption fine structure (EXAFS) analysis based on cumulant expansion or multishell Gaussian model fails for these systems. Therefore, the radial distribution functions (RDFs) around Ag ions were reconstructed using a method based on the direct inversion of the EXAFS expression. The RDFs consist of about eight atoms (oxygens and borons), exhibit a relatively weak temperature dependence, and indicate the presence of strong static disorder. Two main components can be identified in RDFs, located at about 2.3-2.4 A and 2.5-3.4 A, respectively. The chemical types of atoms contributing to the RDF were determined via a simulation of configurationally averaged x-ray absorption near-edge structure (XANES) and EXAFS signals. The immediate neighborhood of Ag contains mostly oxygens while borons dominate at larger distances. The combination of EXAFS and XANES techniques allowed us to determine a more complete structural model than would be possible by relying solely on either EXAFS or XANES alone.Hall effects of the La{sub 0.7}Ce{sub 0.3}MnO{sub 3+{delta}} film, which is believed an electron-doped manganite, have been experimentally studied, and a positive normal Hall coefficient is observed below the Curie temperature when the oxygen content of the film varies in a wide range. These observations may be attributed to the presence of excessive oxygen and composition distribution in the film, which may occur companying tetravalent ion doping. Removing excessive oxygen drives the system into the electron-doping state, however, the resistivity increases monotonically with oxygen loss, and the metal-to-semiconductor transition typical for a hole-doped manganite disappears. These results suggest the determinative role of hole doping for the resistive and magnetic behaviors in La{sub 0.7}Ce{sub 0.3}MnO{sub 3+{delta}}.We studied the influence of the disorder introduced in polycrystalline MgB{sub 2} samples by neutron irradiation. To circumvent self-shielding effects due to the strong interaction between thermal neutrons and {sup 10}B we employed isotopically enriched {sup 11}B which contains 40 times less {sup 10}B than natural B. The comparison of electrical and structural properties of different series of samples irradiated in different neutron sources, also using Cd shields, allowed us to conclude that, despite the low {sup 10}B content, the main damage mechanisms are caused by thermal neutrons, whereas fast neutrons play a minor role. Irradiation leads to an improvement in both upper critical field and critical current density for an exposure level in the range 1-2x10{sup 18} cm{sup -2}. With increasing fluence the superconducting properties are depressed. An in-depth analysis of the critical field and current density behavior has been carried out to identify what scattering and pinning mechanisms come into play. Finally, the correlation between some characteristic lengths and the transition widths is analyzed.The structure of Na{sub 0.5}CoO{sub 2}, the low-temperature insulator that separates the antiferromagnetic and normal metals in the Na{sub x}CoO{sub 2} phase diagram, is studied by high-resolution powder neutron diffraction at temperatures between 10 and 300 K. Profile analysis confirms that it has an orthorhombic symmetry structure, space group Pnmm, consisting of layers of edge-sharing CoO{sub 6} octahedra in a triangular lattice, with Na ions occupying ordered positions in the interleaving planes. The oxygen content is found to be stoichiometric within 1%, indicating that the Na concentration accurately determines the electronic doping. The Na ordering creates two distinct Co sites, in parallel chains running along one crystallographic direction. The differences in their Co-O bond distances and the derived bond valence sums, reflections of the degree of charge ordering in this phase, are very small.The temperature dependence of the local structure of V{sub 2}O{sub 3} in the vicinity of the metal-to-insulator transition (MIT) has been investigated using hard x-ray absorption spectroscopy. It is shown that the vanadium pair distance along the hexagonal c axis changes abruptly at the MIT as expected. However, a continuous increase of the tilt of these pairs sets in already at higher temperatures and reaches its maximum value at the onset of the electronic and magnetic transition. These findings confirm recent theoretical results which claim that electron-lattice coupling is important for the MIT in V{sub 2}O{sub 3}. Our results suggest that the distortion of the symmetry of the basal plane plays a decisive role for the MIT and orbital degrees of freedom drive the MIT via changes in hybridization.We present here ab initio determinations of the nuclear-quadrupole moment Q of hyperfine-probe-nuclear states of three different In isotopes: the 5{sup +} 192 keV excited state of {sup 114}In (probe for nuclear quadrupole alignment spectroscopy), the 9/2{sup +} ground state of {sup 115}In (nuclear magnetic and nuclear quadrupole resonance probe), and the 3/2{sup +} 659 keV excited state of {sup 117}In (perturbed angular correlations probe). These nuclear-quadrupole moments were determined by comparing experimental nuclear-quadrupole frequencies to the electric field gradient tensor calculated with high accuracy at In sites in metallic indium within the density functional theory. These ab initio calculations were performed with the full-potential linearized augmented plane wave method. The results obtained for the quadrupole moments of {sup 114}In [Q({sup 114}In)=-0.14(1) b] are in clear discrepancy with those reported in the literature [Q({sup 114}In)=+0.16(6) b and +0.739(12) b]. For {sup 115}In and {sup 117}In our results are in excellent agreement with the literature and in the last case Q({sup 117}In) is determined with more precision. In the case of Q({sup 117}In), its sign cannot be determined because standard {gamma}-{gamma} perturbed angular correlations experiments are not sensitive to the sign of the nuclear-quadrupole frequency.An original epitaxial system consisting of two ferrimagnetic insulator layers (CoFe{sub 2}O{sub 4} and Fe{sub 3}O{sub 4}) separated by a nonmagnetic metallic layer (Au) has been grown. The transport properties in the current in plane geometry indicate that the conduction of the CoFe{sub 2}O{sub 4}/Au/Fe{sub 3}O{sub 4} trilayer takes place within the thin metallic layer. The giant magnetoresistance (GMR) observed (2.6% at 10 K) is associated to the switching from a parallel to an antiparallel configuration of the magnetization of the two ferrite layers and corresponds to the spin dependence of electron reflection at the interfaces with a large contribution of specular reflections. The increase of the GMR (5% at 10 K) in the symmetrical interface CoFe{sub 2}O{sub 4}/Fe{sub 3}O{sub 4}/Au/Fe{sub 3}O{sub 4} system and the effect of the interface roughness on the GMR confirm the presence of this spin-dependent specular reflection.The effect of externally applied pressure on the magnetic behavior of Cu{sub 2}Te{sub 2}O{sub 5}(Br{sub x}Cl{sub 1-x}){sub 2} with x=0, 0.73, and 1, is investigated by a combination of magnetic susceptibility, neutron diffraction, and neutron inelastic scattering measurements. The magnetic transition temperatures of the x=0 and 0.73 compositions are observed to increase linearly with increasing pressure at a rate of 0.23(2) and 0.04(1) K/kbar, respectively. However, the bromide shows contrasting behavior with a large suppression of the transition temperature under pressure, at a rate of -0.95(9) K/kbar. In neutron inelastic scattering measurements of Cu{sub 2}Te{sub 2}O{sub 5}Br{sub 2} under pressure only a small change to the ambient pressure magnetic excitations were observed. A peak in the density of states was seen to shift from {approx}5 meV in ambient pressure to {approx}6 meV under an applied pressure of 11.3 kbar, which was associated with an increase in the overall magnetic coupling strength.A KH{sub 2}PO{sub 4} (KDP) crystal, irradiated by a 1 MeV hydrogen ion beam to a dose of 10{sup 15} ions/cm{sup 2}, was studied by means of x-ray diffraction (XRD), {sup 1}H nuclear magnetic resonance (NMR), and dielectric constant measurements. The XRD pattern for the a-cut KDP crystal revealed a decrease in the lattice constant along the a axis after the proton irradiation. According to the {sup 1}H NMR spin-lattice relaxation rate measurements, the proton irradiation gave rise to reduction in the activation energy in the paraelectric phase, from 0.42 to 0.28 eV, in agreement with the temperature dependent second moment measurements indicating the proton motion is more activated after the proton irradiation. Besides, analysis of the temperature-dependent dielectric constants using a mean-field approximation revealed a change in the hydrogen bond induced by the proton irradiation.