Large-scale, density functional theory-based screening of alloys for hydrogen evolution

A general scheme for the screening of heterogeneous catalysts using density functional theory (DFT) calculations is presented, and the scheme is illustrated with a search for catalysts for the hydrogen evolution reaction. Simple techniques to estimate the activity of binary surface and bulk alloys for this reaction are described, and several computational tests for stability in reaction environments are presented. Careful application of these activities and stability criteria to a database of DFT calculations on ∼750 binary transition metal alloys leads to the identification of several surface and bulk alloys that are predicted to perform comparably to platinum, the canonical hydrogen evolution catalyst. This study marks the first use of full DFT calculations for high-throughput screening of transition metal catalysts.     

Crisis phenomena in falling liquid films at periodic heat loads

Experimental results on development of crisis phenomena in a falling film of cryogenic liquid at alternating pulse heat release are presented. Experimental data on local temperature evolution along a heat releasing surface are obtained. It is shown that amplitude of heater temperature pulsations depends significantly on the heat flux density and coordinates along the liquid film flow. New experimental data on the critical heat fluxes corresponding to formation of stable dry spots and drying crisis are presented depending on duration of heat release pulses. It is shown that parameters of the forming metastable regular structures and critical drying parameters of the heat-releasing surface are determined by dynamics of the movable boundaries of wetting during self-organization of a system.     

轻原子成像法的建立及其新进展

介绍了利用高分辨电子显微不进行晶体结构分析的一种方法－轻原子成像法的建立过程及其在铜,镍,银等金属的初期氧化产物结构分析中的应用,介绍了利用轻原子成像法的思想解决厚膜上观察表面结构的可能性问题的新进展。     

Stark resonances in disordered systems

We study further the metastable behavior of Metropolis dynamics for the two-dimensional nearest neighbor ferromagnetic Ising model, with positive and small external field, in the limit as the temperature vanishes (see [NS]). We focus on the typical features of the escape (nucleation) from the (metastable) configuration with all spins –1, to the (stable) configuration with all spins +1. Using the reversibility of the process as the main tool, we prove (for the discrete time version of the model) that the first step of a typical escaping path is the time reverse of a typical time evolution of a shrinking subcritical rectangular droplet, which is one slice smaller than a critical droplet. This subcritical droplet then evolves in a time of order 1 to a critical droplet, which finally grows with features described in [NS].Work partially supported by the Brazilian CNPq and by the American NSF, under grant DMS91-00725     

A 2-dimensional detector with high spatial and temporal resolution for metastable rare gas atoms

We describe a detector for metastable rare gas atoms which allows the investigation of transverse atomic beam distributions on the single atom level with lateral dimensions of 1 m, which occur frequently in the field of atom optics. In contrast to existing detection techniques, the conversion step from the metastable atom to an electron is separated from the charge amplification to improve spatial resolution. The conversion is performed at a metal surface, which is followed by an electron-optical system imaging the electron distribution with a proper magnification onto a single electron detection unit. The spatial resolution that we achieve with this technique is on the order of 1 m, the temporal resolution on the order of 1 s. The application of the detector for atom interferometry is discussed. Received: 22 May 1996 / Revised version: 21 June 1996     

A study of morphological and compositional evolution of nanoprecipitates in the Zr–Nb system and their transformational behavior

The metastable transformational behavior (both martensitic and omega) along with compositional and morphological evolution of bcc β precipitates, dispersed in the hcp α matrix of a Zr–1 wt% Nb alloy, were studied as a function of temperature and time. The evolution of the chemical composition of the β phase suggested preference towards metastable compositions having Nb content higher than the equilibrium value. Thermodynamic analysis showed that the metastable chemical compositions are the driving force for the nucleation of such β precipitates. The β to martensite transformation was observed to be possible only if β precipitate size exceeded a critical value of 160?nm. Micromechanical modeling was performed to estimate the critical size of β precipitate required to induce martensite transformation and the model predictions were in close agreement with the experimental observations. The omega transformation, on the other hand, showed less size dependence.     

基于无导数优化方法的数值模式误差估计

初始场误差和模式误差是制约数值预报准确率的两个关键因素,本文主要考虑利用历史观测资料实现时空演变的模式误差的估计问题.通过把模式误差综合考虑成为准确模式中的未知项,把历史资料看作是带有未知项的准确模式的特解,构造了求解时空演变的模式误差项的反问题及其最优控制问题.给出了一个解决最优控制问题的无导数优化方法,该方法的优点是不需要建立原数值模式的切线性模式与伴随模式,它只需在增加一个外强迫项的基础上运行原数值模式即可实现模式误差项的最优估计.关于Burgers方程的算例表明,无论模式的初始状态是否准确已知,无导数优化方法都能有效解决时空演变的模式误差的最优估计问题,它为实际业务模式利用历史数据提取模式误差信息并显著地改进预报效果提供了一种方便可行的数值方法与理论依据.     

Capillarity-Induced Surface Morphologies

Surface energetics is reviewed including expressions for the chemical potential of a curved surface element and the Legendre transform relation between the projected surface free energy as a function of orientation and the Wulff equilibrium shape. A well known equation is derived describing surface evolution by surface diffusion, assuming local equilibrium. Solutions are reviewed including a decaying sinusoid and a developing thermal groove. Breakdown of local equilibrium is considered. The structure, energetics and dynamics of steps on a vicinal surface are discussed. Facet sizes on the Wulff shape and the surface profile at the edge of a facet are related to the step self and interaction free energies respectively. Fourier analysis of step fluctuations is described, revealing the underlying transport processes. Analysis of the decay of a sinusoidal profile on a vicinal surface in terms of step behavior is given. Finally, examples are reviewed of surface evolution below the roughening temperature T _R in which case facets move by the lateral spreading of steps. Results differ greatly from those of the continuum theory applicable above T _R.     

Rational reduction of periodic propagators for off-period observations

Many common solid-state nuclear magnetic resonance problems take advantage of the periodicity of the underlying Hamiltonian to simplify the computation of an observation. Most of the time-domain methods used, however, require the time step between observations to be some integer or reciprocal-integer multiple of the period, thereby restricting the observation bandwidth. Calculations of off-period observations are usually reduced to brute force direct methods resulting in many demanding matrix multiplications. For large spin systems, the matrix multiplication becomes the limiting step. A simple method that can dramatically reduce the number of matrix multiplications required to calculate the time evolution when the observation time step is some rational fraction of the period of the Hamiltonian is presented. The algorithm implements two different optimization routines. One uses pattern matching and additional memory storage, while the other recursively generates the propagators via time shifting. The net result is a significant speed improvement for some types of time-domain calculations.     

Effect of reduced cooperativity on growth-induced polarity formation: a comparison between different growth models

We investigate the influence of the growth process on macroscopic polarity formation in molecular crystals consisting of polar molecules with two directional states. Specifically, layer-by-layer growth is compared with growth along surface steps, and growth at kink sites. Idealized models for these growth processes are presented, being characterized by the thermal equilibrium formation of a domain of molecules on the surface, ranging from an entire adlayer to a single molecule only (reduced cooperativity). Longitudinal and lateral Ising-type nearest neighbour interactions are taken into account. Formerly attached and thermalized molecules are kept frozen upon growth and therefore, bulk polarity results. Growth models are studied by means of Monte Carlo simulations. Results show that a reduced cooperativity between neighbouring molecules on the crystal surface increases the probability of orientational disorder. However, in the asymptotic limit of infinite growth and for sufficiently strong longitudinal couplings, phenomenologically, evolution of polarity for step and kink growth remains the same as for layer-by-layer growth, being mainly a thermodynamically driven process. Despite their strong out-of-equilibrium character, step and kink growth processes feature a continuous phase transition as layer-by-layer growth and are reasonably well described by an effective lateral coordination number within a mean field approach.     

Metastable surface alloys produced by ion implantation,laser and electron beam treatment

Ion Implantation, Laser and Electron-beam Treatment (LET) of metals have been employed extensively to produce metastable surface alloys. Recent published work on implanted alloys is reviewed first. The dilute implanted alloys (solute concentration <10 at. %) are shown to lead to crystalline metastable solid solutions. At higher solute concentrations, an amorphous phase has been observed for several binary systems and recently for a ternary system. The physical mechanisms at play, are discussed in detail. A review of the surface alloys produced by LET of metals is then presented—with an emphasis on the mechanisms involved. In particular, general criteria governing formation of metastable solid solutions under LET are proposed and shown to have excellent agreement with available data on metals and Si.     

Numerical investigation of the submonolayer growth and relaxation of stepped Ag (110) and Au (110) surfaces

The terrace width distribution (TWD) as well as the adatom and island densities for some stepped fcc?(110) surfaces with parallel and equidistant steps of equal stiffness are studied by means of kinetic Monte Carlo simulations. Reliable energy barriers for surface diffusion are used. They have been calculated by means of many-body potentials derived within the second moment approximation to the tight-binding model. The effects of the temperature, atom deposition flux and surface diffusion on quantities of interest in the early stage of the surface evolution process have been singled out. In most cases, linear, logarithmic and power-law behaviors are recovered for the evolution of the step width and terrace defects. The TWD is well described by the Gaussian distribution (GD) in the domain of temperature investigated but deviates from the Generalized Wigner Distribution (GWD).     

A two-dimensional multispecies fluid model of the plasma in an ACplasma display panel

A time dependent, two-dimensional model for simulating the plasma evolution in an AC plasma display panel (AC-PDP) is described. Reaction-convection (mobility)-diffusion equations for charged particles and excited heavy neutral species are solved along with Poisson's equation, a radiation transport equation, a surface charge buildup equation, and an external L-R-C circuit equation using a fully implicit numerical method. Electron-driven rate coefficients are computed with a 0-D Boltzmann solver in the local field approximation. For studying the particle dynamics in pure helium, we consider a reduced model in which radiation transport is ignored and the excited species manifold is collapsed to composite metastable and excited states. The model predictions of breakdown voltage are quite sensitive to the value of the secondary electron emission coefficient assumed and the uncertainties in the electron-driven reaction rates. An initial comparison between the model predictions and I-V measurements from a specially constructed helium-filled panel is made with qualitatively similar behavior. The lack of quantitative agreement can be explained by a combination of uncertainties in the model input data and uncertainty in the initial surface charge state in the experiments     

Kinetics of surface segregation in alloys

The kinetics of surface segregation in ordering alloys are studied with the help of a multilayer model in slabs of different thicknesses. The time evolution of the concentrations of atomic layers perpendicular to the (100) planes of an AB-type BCC ordering alloy (CoFe) are calculated. As a result of the competition between the surface segregation of A atoms and ordering in the bulk, a metastable configuration with two anti-phase boundaries (APB) inside the slab, with odd numbers of layers, was obtained if we started from an ordered initial state with B atoms on the free surfaces (B-termination). The effect of the temperature was also investigated for a slab with 41 layers and from the calculation of the free energies of the metastable and stable states it was shown that the metastable state can exist below T₁ = 0.95T_c, where T_c is the critical temperature of the order-disorder transition in bulk. It was obtained that T₁ decreases with decreasing thickness of the slab, while the difference of free energies of the metastable and stable states slightly increases. The effect of the slab thickness is a typical size effect: the time necessary to reach the steady state decreases with decreasing number of layers.     

Elastic interaction of surface steps: effect of atomic-scale roughness

Elastic interactions of atomic steps can greatly impact surface morphology. Recent atomistic calculations and experimental observations find the standard dipole model of steps is valid only for very large step separations. In this Letter, a new model is presented that displays remarkable agreement with atomistic predictions for step separations larger than just a few step heights. It is shown that the interaction energy of steps exhibits a novel intermediate-ranged behavior and that, for particular systems, step interactions switch from repulsive to attractive as separation distance decreases.     

基于目标识别的多传感器图像信息融合技术

本文针对目标识别问题，论述了多传感器目标属性融合技术。包括目标属性融合概念、原理、处理结构、算法及应用举例。指出了多传感器目标属性融合中存在的主要问题及解决方法，并预测了发展趋势     

Hadron production in relativistic nuclear collisions: thermal hadron source or hadronizing quark-gluon plasma?

Measured hadron yields from relativistic nuclear collisions can be equally well understood in two physically distinct models, namely a static thermal hadronic source vs. a time-dependent, nonequilibrium hadronization off a quark-gluon plasma droplet. Due to the time-dependent particle evaporation off the hadronic surface in the latter approach the hadron ratios change (by factors of ) in time. Final particle yields reflect time averages over the actual thermodynamic properties of the system at a certain stage of the evolution. Calculated hadron, strangelet and (anti-)cluster yields as well as freeze-out times are presented for different systems. Due to strangeness distillation the system moves rapidly out of the , plane into the -sector. Strangeness to baryon ratios prevail during a considerable fraction (50%) of the time evolution (i.e. -droplets or even -droplets form the system at the late stage: The possibility of observing this time evolution via two-particle correlations is discussed). The observed hadron ratios require MeV and MeV. If the present model is fit to the extrapolated hadron yields, metastable hypermatter can only be produced with a probability for . Received: 15 April 1997 / Revised version: 5 June 1997     

Cooperative stochastic behavior in the onset of localized corrosion

Stochastic temporal and spatiotemporal models of metastable pitting on a metal surface are presented. A stochastic reaction-diffusion model accounts for the effects of local changes in concentration, potential drop, and oxide film damage on the nucleation of subsequent events. The cooperative interactions among events can lead to the formation of clusters of metastable pits and to an explosive growth in the total number of pits. Recent progress in the studies of such phenomena is reviewed. New results based on a mean-field analysis of the model and numerical simulations on critical nucleation effects are reported.