Dynamic anisotropy and heterogeneity of polystyrene thin films as studied by inelastic neutron scattering

We studied the dynamic anisotropy and heterogeniety of polystyrene thin films in glassy state with inelastic neutorn scattering. Adjusting the scattering vector to the directions parallel and perpendicular to the film surface, we observed the elastic scattering intensities as a function of temperature. It was found for the 200 A film that the elastic intesity decreased with increasing temperature more rapidly in the perpendicular direction than in the pararell direction, showing the higher mobility in the perpendicular direction. However, such dynamical anisotropy was not observed in the 1000 A film. The decrease in the mobility was observed with the film thickness in both the directions. These results were explained in terms of an interface hard layer. We also evelauated the dynamical heterogeniety from the non-Gaussian parameter A0, which increased with decreasing the film thickness, showing the increase in the dynamical heterogeneity. Assuming a simple bi-layer model consisting of the interface hard layer and the bulk-like layer, we analyzed the thickness dependence of the non-Gaussian parameter A0 and the mean square displacement (u2) to find that the hard layer has a thickness of approximately 130 A and a mean square displacement of approximately 0.018 A2 at 230 K.     

Quantum transport in mesoscopic 3He films: experimental study of the interference of bulk and boundary scattering

We discuss the mass transport of a degenerate Fermi liquid ^{3}He film over a rough surface, and the film momentum relaxation time, in the framework of theoretical predictions. In the mesoscopic regime, the anomalous temperature dependence of the relaxation time is explained in terms of the interference between elastic boundary scattering and inelastic quasiparticle-quasiparticle scattering within the film. We exploit a quasiclassical treatment of quantum size effects in the film in which the surface roughness, whose power spectrum is experimentally determined, is mapped into an effective disorder potential within a film of uniform thickness. Confirmation is provided by the introduction of elastic scattering centers within the film. The improved understanding of surface roughness scattering may impact on enhancing the conductivity in thin metallic films.     

First inelastic neutron scattering studies on thin free standing polymer films

Glass transition studies in free standing polymer films have revealed values of the transition temperature, T(g), which were substantially reduced below the bulk for sufficiently thin films. Here we report on the preparation of two stacks of free standing polystyrene films: 70 films with a thickness of h approximately 107 nm and 140 films with h approximately 55 nm with equivalent total sample thicknesses of approximately 7.5 microm. We have performed the first measurements on such samples using inelastic neutron scattering, and demonstrate that inelastic neutron scattering experiments, performed on the time-of-flight spectrometer IN6 and the backscattering spectrometer IN16 at the Institut Laue-Langevin, are feasible.     

Opposite spin asymmetry of elastic and inelastic scattering of nonequilibrium holes injected into a ferromagnet

The spin asymmetry of elastic and inelastic scattering of nonequilibrium holes injected into Co thin films is examined using a p-type magnetic tunnel transistor. Spin-dependent transmission yields a positive or negative magnetocurrent depending on Co thickness and hole energy. Up to a critical thickness of about 3 nm, (quasi)elastic scattering dominates with a short attenuation length (<1 nm) and preferential attenuation of holes in the majority spin bands, consistent with spin-wave emission. At a larger Co thickness, inelastic scattering dominates with a larger attenuation length ( approximately 4 nm) and opposite spin asymmetry.     

Simultaneous characterization of protein coated iron oxide nanoparticles with nuclear inelastic scattering and atomic force microscopy

Bovine serum albumin coated magnetic iron oxide nanoparticles (IONPs), which were synthesized using a co-precipitation method with ⁵⁷Fe have been subject to a combined study using atomic force microscopy (AFM) and nuclear inelastic scattering (NIS). The obtained partial density of vibrational states (pDOS) shows evidence for lattice stiffening and a pronounced mode at 23 meV compared to thin film magnetite at room temperature.     

Enhanced scattering from a thin film with one-dimensional disorder

This paper deals with a TE plane wave scattering from a thin film with one-dimensional disorder by means of the stochastic functional approach. The thin film is one-dimensionally inhomogeneous in the horizontal direction with infinite extent, and is homogeneous in the vertical direction with finite thickness. Based on an approximate wavefield representation in terms of a Wiener–Hermite expansion in a preceding paper (Tamura et al., 2004, Waves in Random Media, 14, 435–465), the first- and second-order incoherent scattering cross-sections are presented in explicit forms and scattering properties are discussed. The scattering properties vary entirely with the film thickness. In a case where the thickness is smaller than a few wavelengths in the thin film, enhanced scattering and associated enhanced scattering may appear as sharp peaks or dips on the second-order incoherent scattering distribution if the thin film has guided wave modes. When the thickness becomes sufficiently larger than the wavelength inside the film, a new enhanced scattering phenomenon appears as gentle peaks on the second-order incoherent scattering distribution in four special directions. Such four directions are the directions of forward scattering, specular reflection, backscattering, and the symmetrical direction of forward scattering with respect to the normal of the film surface.The first-order incoherent scattering occurs distinctly in four such directions. Such enhanced scattering is independent of the existence of the guided wave modes inside the thin film, and deeply relates to the structure of the thin film with one-dimensional disorder that has infinite correlation in the vertical direction. For SiC and glass thin films having one-dimensional disorder with a Gaussian correlation and three types of exponential correlation, the first- and second-order incoherent scattering cross-sections are illustrated in figures. The narrow enhanced scattering peaks appear for the glass film in a thin case. The gentle enhanced peaks turn up for both the SiC and glass films in a thick case. Furthermore, the optical theorem is calculated for several cases. It is then found that the error of the optical theorem decreases and the performance of the wavefield is improved by taking into account the second-order incoherent scattering.     

Investigation of interface roughness cross-correlation properties of optical thin films from total scattering losses

The interface roughness and interface roughness cross-correlation properties affect the scattering losses of high-quality optical thin films. In this paper, the theoretical models of light scattering induced by surface and interface roughness of optical thin films are concisely presented. Furthermore, influence of interface roughness cross-correlation properties to light scattering is analyzed by total scattering losses. Moreover, single-layer TiO₂ thin film thickness, substrate roughness of K9 glass and ion beam assisted deposition (IBAD) technique effect on interface roughness cross-correlation properties are studied by experiments, respectively. A 17-layer dielectric quarter-wave high reflection multilayer is analyzed by total scattering losses. The results show that the interface roughness cross-correlation properties depend on TiO₂ thin film thickness, substrate roughness and deposition technique. The interface roughness cross-correlation properties decrease with the increase of film thickness or the decrease of substrates roughness. Furthermore, ion beam assisted deposition technique can increase the interface roughness cross-correlation properties of optical thin films. The measured total scattering losses of 17-layer dielectric quarter-wave high reflection multilayer deposited with IBAD indicate that completely correlated interface model can be observed, when substrate roughness is about 2.84 nm.     

Transmission of high-frequency phonons through thin glass films

By means of phonon spectroscopy we measured the transmission of high-frequency phonons through thin glass films in the frequency range from 100 to 300 GHz. The films were prepared by thermal oxydation of silicon single crystals. Our data obtained from films with different thicknesses suggest that the observed phonon attenuation is due to scattering processes at the silicon-glass interface and not to a bulk effect in the glass film. The phonon mean free path at 300 GHz turns out to be larger than 4microm. We find evidence for the absence of inelastic scattering processes.     

非晶态Se薄膜的自发晶化研究

利用真空热蒸镀的方法制备了非晶Se薄膜,测试了稳定的非晶Se薄膜,不稳定的非晶Se薄膜和初始自发晶化的非晶Se薄膜的透射率光谱和拉曼光谱,对透射率光谱曲线进行了拟合,计算了薄膜的厚度和折射率随波长的变化关系。在自我晶化过程中,Se薄膜折射率逐渐增大;随波长增大,折射率则减小,初始自发晶体的Se薄膜中,出现标志Se8环和链的结构,不完整的环和链结构在自发晶化过程中得到了增强。     

Crystallization Kinetics of Lamellar Crystals Confined in Polymer Thin Films

We used dynamic Monte Carlo simulations to investigate the crystallization kinetics of flat-on lamellar polymer crystals in variable thickness films. We found that the growth rates linearly reduced with decreasing film thickness for the films thinner than a transition thickness d_t , while they were constant for the films thicker than d_t . Moreover, the mean stem lengths (crystal thickness) we calculated decreased with film thickness in a similar way to the growth rates, and the intramolecular crystallinities we calculated confirmed the film thickness dependence of the crytsal thickness. Besides, the crystal melting rates in thin films were calculated and increased with decreasing film thickness. We proposed a new interpretation on the film thickness dependence of the crystal growth rate in thin films, suggesting that it is dominated by the crystal thickness in terms of the driving force term (l–l _min) expressed by Sadler, rather than the chain mobility based on experiments. The crystal thickness can determine whether a crystal grows or melts in a thin film at a fixed temperature, indicating the reversibility between the crystal growth and melting.     

Stability of thermoresponsive methylcellulose thin film: x‐ray reflectivity study

Methylcellulose (MC), a thermoreversible polymer, was fabricated as thin films into silicon substrates and characterized by x‐ray reflectivity (XRR) measurements for its stability with time and heating. XRR data from the as‐is thin films showed good agreement with the single‐layer model on top of a substrate from Parratt's formalism. Data fitting showed that the density of the thin films is slightly higher than the reported value by manufacturers. Interface roughness values indicate good wetting of the polymer onto the substrate. Heating the thin films at the phase transition temperatures and quenching them to room temperature showed no significant changes in the thin film parameters before and after heating. This showed the thermal stability and/or thermoreversibility of the film. Diffuse scattering measurements also showed no significant changes in the lateral structure of the film with heating and quenching. XRR measurements done on fabricated thin films stored for a month showed a slight increase in the film thickness which could be due to the hygroscopic nature of the polymer. Vacuum heating of the stored thin films at 100 °C for 1 h slightly decreased the thickness, but it has been found that other parameters such as density and surface/interface roughness show good thermal stability. Copyright © 2009 John Wiley & Sons, Ltd.     

InN thin film lattice dynamics by grazing incidence inelastic x-ray scattering

Achieving comprehensive information on thin film lattice dynamics so far has eluded well established spectroscopic techniques. We demonstrate here the novel application of grazing incidence inelastic x-ray scattering combined with ab initio calculations to determine the complete elastic stiffness tensor, the acoustic and low-energy optic phonon dispersion relations of thin wurtzite indium nitride films. Indium nitride is an especially relevant example, due to the technological interest for optoelectronic and solar cell applications in combination with other group III nitrides.     

Enhanced scattering from a thin film with one-dimensional disorder

This paper deals with a TE plane wave scattering from a thin film with one-dimensional disorder by means of the stochastic functional approach. The thin film is one-dimensionally inhomogeneous in the horizontal direction with infinite extent, and is homogeneous in the vertical direction with finite thickness. Based on an approximate wavefield representation in terms of a Wiener-Hermite expansion in a preceding paper (Tamura et al., 2004, Waves in Random Media, 14, 435-465), the first- and second-order incoherent scattering cross-sections are presented in explicit forms and scattering properties are discussed. The scattering properties vary entirely with the film thickness. In a case where the thickness is smaller than a few wavelengths in the thin film, enhanced scattering and associated enhanced scattering may appear as sharp peaks or dips on the second-order incoherent scattering distribution if the thin film has guided wave modes. When the thickness becomes sufficiently larger than the wavelength inside the film, a new enhanced scattering phenomenon appears as gentle peaks on the second-order incoherent scattering distribution in four special directions. Such four directions are the directions of forward scattering, specular reflection, backscattering, and the symmetrical direction of forward scattering with respect to the normal of the film surface.The first-order incoherent scattering occurs distinctly in four such directions. Such enhanced scattering is independent of the existence of the guided wave modes inside the thin film, and deeply relates to the structure of the thin film with one-dimensional disorder that has infinite correlation in the vertical direction. For SiC and glass thin films having one-dimensional disorder with a Gaussian correlation and three types of exponential correlation, the first- and second-order incoherent scattering cross-sections are illustrated in figures. The narrow enhanced scattering peaks appear for the glass film in a thin case. The gentle enhanced peaks turn up for both the SiC and glass films in a thick case. Furthermore, the optical theorem is calculated for several cases. It is then found that the error of the optical theorem decreases and the performance of the wavefield is improved by taking into account the second-order incoherent scattering.     

Influence of film structure on the surface vibrations of Co/Au(111)

The vibrational properties of thin Co layers on a Au(111) surface have been probed by means of inelastic He-atom scattering at primary beam energies between 25 and 67 meV. The observed dependence of the Au(111) Rayleigh mode intensity on Co coverage and annealing temperature as well as the only weak evidence for phonons of the Co film can be explained in terms of the particular growth mode of Co on the Au(111) surface.     

Energy relaxation of hot electrons and inelastic collision time in thin metal films at low temperatures

In a sandwich consisting of a thin Au film and a thin Bi film insulated by a 500 Å SiO layer the electrons of one film are heated above the lattice temperature while in the other film they are kept in thermal equilibrium temperature while in the other film they are kept in thermal equilibrium with the phonons. By measuring the magnetoresistance of both films we obtain the temperature difference between electrons and phonons from which we imply the energy-relaxation time τ_ϵ from 0.3 K to 2 K. We find that electron-phonon scattering determines τ_ϵ and, above 5 K, also the inelastic collision time τ_i obtained from weak localization theory in thermal equilibrium.     

Growth Rates of Edge-on Lamellar Crystals Confined in Polymer Thin Films

The growth rates of edge-on lamellar polymer crystals in variable thickness films were investigated in terms of dynamic Monte Carlo (MC) simulations. The growth rates linearly decreased with decreasing film thickness for the thinner films and were nearly constant for the thicker films. The mean stem lengths (crystal thickness) were also constant in different thickness films. The crystal widths parallel to the film thickness increased more slowly with increasing film thickness in the thinner films than that in the thicker films, indicating they were restrained by the film thickness. We propose that the growth rate of edge-on lamellar crystals in thin films is dominanted by the crystal width in the thinner films and by the crystal thickness in the thicker films; the variation of the film thickness can change the three-dimensional shape of the crystal growth front, also affecting the growth rate of the edge-on lamellar crystal.     

X-ray reflectivity studies on glass transition of free standing polystyrene thin films

We have studied thermal expansion of free standing polystyrene thin films using X-ray reflectivity to elucidate the glass transition temperature and the thermal expansivity. We found that the glass transition temperature T_g decreased with the film thickness, depending on molecular weight. The reduction in the free standing films is much larger than in the supported films on Si substrate, suggesting that some segmental motions are activated due to free surfaces on both sides in the free standing films. We also found that the thermal expansivity in the glass and the melt decreased with the film thickness. This decrease must be attributable to chain confinement effects.     

Mode-selected electron-phonon coupling in superconducting Pb nanofilms determined from He atom scattering

The electron-phonon coupling (EPC) strength for each phonon mode in superconducting Pb films is measured by inelastic helium atom scattering (IHAS). This surprising ability of IHAS relies on two facts: (a) In ultrathin metal films, the EPC range exceeds the film thickness, thus enabling IHAS to detect most film phonons, even 1 nm below the surface; (b) IHAS scattering amplitudes from single phonons are shown, by first-principle arguments, to be proportional to the respective EPC strengths. Thus IHAS is the first experiment providing mode-selected EPC strengths (mode-lambda spectroscopy).     

Effect of electrically degenerated layer on the carrier transport property of ZnO epitaxial thin films

ZnO films were prepared on (1 1 1) YSZ and (0 0 0 1) sapphire by pulsed laser deposition method. Effect of lattice mismatch on the carrier transport properties of ZnO epitaxial thin films was investigated. The carrier mobility of the ZnO films on YSZ was larger than that of ZnO/sapphire due to smaller lattice mismatch when the thickness was below 150 nm. The effect of electrically degenerated layer on the carrier transport property increased with decreasing the film thickness of ZnO film. The carrier density and electron mobility of 20 nm-thick-ZnO film on either substrate were regardless of the temperature. We concluded that the dominant carrier scattering mechanism in ZnO ultra thin films is double Schottky barriers at the grain boundary and that their height depends on the carrier concentration.     

Applicability of magic angle for angle-resolved X-ray photoelectron spectroscopy of corrugated SiO2/Si surfaces: Monte Carlo calculations

In several earlier works, the “magic angle” has been introduced in overlayer thickness estimation from angle-resolved X-ray photoelectron spectra as a practical tool for suppressing experimental errors induced by surface corrugation. We analyse the applicability of the “magic angle” in Monte Carlo calculations of random as well as non-random corrugated silicon surfaces covered by thin silicon dioxide films, accounting for (a) electron inelastic and elastic scattering events, (b) the shadowing of photoelectrons, and (c) the differences between microscopic and macroscopic electron emission geometry. It is shown that the “magic angle” value varies with the type of surface roughness, overlayer thickness, surface contamination, an uneven overlayer thickness and electron inelastic surface excitations.