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We present an overview of the theory developed over the last few years to describe the crystallization of amorphous solids. The microstructure of the crystallizing solid is described in terms of the grain size distribution (GSD). We propose a partial differential equation that captures the physics of crystallization in random nucleation and growth processes. The analytic description is derived for isotropic and anisotropic growth rates and allows for the analysis of different stages of crystallization, from early to full crystallization. We show how the timedependence of effective nucleation and growth rates affect the final distribution. In particular, we demonstrate that for cases described by the Kolmogorov-Avrami-Mehl-Johnson (KAMJ) model applicable to a large class of crystallization processes a lognormal type distribution is obtained at full crystallization. The application of the theory to the crystallization of silicon thin films is discussed.
A “0-0 type” multiferroic BaTiO3-NiFe2O4 (BT-NF) composite thin film was prepared on SrRuO3/(La,Sr)MnO3/CeO2/YSZ/Si(001) substrate using pulsed laser deposition (PLD). Epitaxial growth of the film was confirmed using x-ray pole figure measurements. Cross-sectional TEM observations revealed that the crystal structure and morphology of the BT-NF composite thin film depends on the oxygen pressure during deposition. The film deposited at 1.0×10-2 Torr has smaller grains than that deposited at 1.0×10-1 Torr. The magnetic and ferroelectric properties of BT-NF composite thin film were correlated with the microstructure that was controlled by oxygen pressure during deposition. The film deposited at 1.0×10-2 Torr had paramagnetic properties with less polarization than the film deposited at 1.0×10-1 Torr.
The ion beam synthesis of Pb nanoparticles (NPs) in silica/silicon films is studied in terms of the combination of a two-step annealing process consisting of a low temperature long time aging treatment followed by a high temperature short time furnace annealing. The samples are analyzed through Rutherford Backscattering Spectrometry and Transmission Electron Microscopy. The aging process leads to the suppression of the classical homogeneous nucleation of metallic Pb NPs in the silica, thus promoting Pb redistribution during the high temperature annealing. This causes the formation of dense bi-dimensional NP arrays located at the silica-silicon interface, presenting small size dispersion.
The growth of epitaxial semiconductor nanostructures and films at low temperatures is important for semiconductor technology because it allows the possibility of monolithically integrating different high-performance single-crystalline semiconductor structures directly onto low cost technologically important substrates. At sufficiently low temperatures this can enable, for example, Si or Ge device fabrication on flexible substrates such as plastics. We have studied the reduced-temperature liquid-mediated growth of Ge nanostructures and films on crystalline template layers on non-single-crystalline substrates in a low-pressure chemical vapor deposition (LPCVD) system. The heteroepitaxial process is implemented by the Au seeded vapor-liquidsolid (VLS) catalytic growth technique with germane below 400 ºC. Crystalline template layers were prepared with ion-beam-assisted-deposition (IBAD) texturing and electron-beam evaporation on glass substrates. A thin layer of e-beam evaporated Au forms the catalyst layer, upon which we grew Ge films at 386 ºC. Scanning electron microscopy and x-ray diffraction results indicated that both Ge islands and nanowires grew heteroepitaxially on the crystalline template layers on glass substrates with good alignment over large areas.
Carbon nanotubes (CNTs) exhibit liquid crystalline order and their nematic director couples to the one of low molecular weight liquid crystals. Here we explore the interactions between CNTs and the smectic liquid crystal phase of a polymer and the possibility for a similar coupling in this system. Isotactic Polypropylene (iPP) and iPP/CNTs nanocomposites were made in solution with varying CNT concentrations and hot pressed into 50-100μm thick films. The pure iPP and iPP/CNT films were then sheared at one rotation per second in the melt state. Shearing continued as the temperature was decreased from 200°C to 145°C to induce a smectic liquid crystal phase. The sheared samples were analyzed using polarized optical microscopy, Two Dimensional Microscopic Transmission Ellipsometry (2D-MTE) and Two Dimensional Wide Angle X-Ray Scattering (2D-WAXS). During shearing we detected a sudden increase of birefringence at 151°C in the samples, higher than the iPP crystallization temperature, indicating liquid crystalline ordering. The samples were then crystallized at 135°C for 30 minutes. We measured anisotropic 2D-WAXS patterns of the samples that contained CNTs, indicating strong ordering of the crystals. Upon reheating, we measured birefringence at temperatures higher than the melting endotherm for the iPP crystals, using polarized microscopy, which indicates that some smectic order still persists in the samples, even after crystallization and complete melting of all crystals. Our results indicate that CNTs couple to the smectic phase of iPP, improve its order upon shearing and the crystals created after the formation of the oriented smectic phase are strongly aligned parallel to the direction of shearing.
In order to deposit YBCO coated conductor with high critical current densities on rolling assisted biaxially textured Ni-W tapes, this paper has systematically studied the influence of deposition conditions on the orientation, in-plane texture and surface morphology of buffers and superconducting layers. It was found that the crystalline alignment and the in-plane texture of cerium oxide cap-layers were well improved by optimizing deposition parameters. The full width at half maximum of phi-scan x-ray diffraction peaks were reduced from original values of 7-8 degrees to 5-6 degrees. A high critical current density of 4.6×106 A/cm2 has been achieved on optimized buffer layers. This value is comparable with the critical current density of YBCO thin films deposited on single crystalline substrates.
The most frequently used characterization technique for biaxial texture formation in thin films is x-ray pole figure analysis. However, x-rays interact weakly with matter and can penetrate a few microns deep into the film. The texture obtained by x-rays is therefore an average texture from the entire thickness of the film. As the texture of a film often changes during growth, information on the basic mechanisms that control the final texture is often lost. In contrast electrons interact strongly with matter and they have very limited penetration and escape depths of a few nm. In this paper we will show how we can use our newly developed reflection high energy electron diffraction (RHEED) surface pole figure technique to probe the surface texture evolution of the growth front from the initial stage (nm thick) to the later stage. The RHEED pole figure technique is a surface-sensitive technique that allows us to obtain information on the dynamic behavior of texture evolution of the growth front during film deposition. We shall explain the principle, measurement, and construction of such RHEED surface pole figures. An example of the biaxial texture evolution of CaF2 due to the atomic shadowing effect during oblique angle deposition is described.
Organized nanostructures are formed after irradiation of layers of randomly aligned single-wall carbon nanotube (SWNT)-polymer composites by a Ti:Sapphire 775 nm laser with a 150 fs pulse at fluences near 0.1 J/cm2. At varying peak fluences morphology is seen where the tubes are ejected from the substrate or formed into long, parallel structures of SWNT’s. These structures have been created on both glass substrates and carbon grids. Transmission Electron Microscopy (TEM) and Scanning Electron Microscopy (SEM) investigation of the structures reveal that they are composed of bundled nanotubes typically 400 nm – 1 micron long. Large-area laser patterning of the film allows for structuring of the film without detrimental decreases in conductivity.