O在Au(111)表面吸附的密度泛函理论研究

应用密度泛函理论，本文系统地研究了O在Au(111)表面上的吸附能、吸附结构、功函数、电子密度和投影态密度，给出了覆盖度从0.11ML到1.0ML的范围内，O的吸附特性随覆盖度变化的规律.研究发现O的稳定吸附位为3重面心立方(fcc)洞位，O在fcc洞位的吸附能对覆盖度比较敏感，其值随着覆盖度的增加而减小；O诱导Au(111)表面功函数的变化量与覆盖度成近线性关系，原因是Au表面电子向O偏移，形成表面偶极子；O—Au的相互作用形成成键态和反键态，且反键态都被占据，造成O—Au键很弱，O吸附能较小. 关键词： 表面吸附 Au(111)表面 密度泛函理论 电子特性     

极性晶体中强耦合表面磁极化子特性

研究极性晶体中表面磁极化子的特性。采用Huybrechts线性组合算符和幺正变换方法,导出了晶体中强耦合表面磁极化子处于基态的振动频率和有效哈密顿量,讨论了坐标z的两种极限情况,对RbCl晶体进行了数值计算。结果表明:振动频率和平行有效哈密顿量随磁场的增加而增大。     

Constructing Invariant Fairness Measures for Surfaces

The paper proposes a rational method to derive fairness measures for surfaces. It works in cases where isophotes, reflection lines, planar intersection curves, or other curves are used to judge the fairness of the surface. The surface fairness measure is derived by demanding that all the given curves should be fair with respect to an appropriate curve fairness measure. The method is applied to the field of ship hull design where the curves are plane intersections. The method is extended to the case where one considers, not the fairness of one curve, but the fairness of a one parameter family of curves. Six basic third order invariants by which the fairing measures can be expressed are defined. Furthermore, the geometry of a plane intersection curve is studied, and the variation of the total, the normal, and the geodesic curvature and the geodesic torsion is determined.     

Cosmic dust and our origins

The small solid particles in the space between the stars provide the surfaces for the production of many simple and complex molecules. Processes involving the effects of ultraviolet irradiation of the thin (hundredth micron) mantles are shown to produce a wide range of molecules and ions also seen in comets. Some of the more complex ones inferred from laboratory experiments are expected to play an important role in the origin of life. An outline of the chemical evolution of interstellar dust as observed and as studied in the laboratory is presented. Observations of comets are shown to provide substantial evidence for their being fluffy aggregates of interstellar dust as it was in the protosolar nebula, i.e. the interstellar cloud which collapsed to form the solar system. The theory that comets may have brought the progenitors of life to the earth is summarized.     

烷基硫酸盐表面张力的量子化学研究

用AMl量子化学计算法优化了十三烷基硫酸根阴离子和——CH3在不同取代位的十二烷基硫酸根阴离子的几何构型，得到最优构型时最高占据分子轨道能级EHOMO、最低空轨道能级ELUMO、电子能量Eele和偶极矩μ等数据．将这些电子结构数据分别与表面张力相拟合，得到很好的相关性。文中讨论了——CH3在不同位置取代对表面张力的影响。     

Time delay as a key to apoptosis induction in the p53 network

A feedback mechanism that involves the proteins p53 and mdm2, induces cell death as a controlled response to severe DNA damage. A minimal model for this mechanism demonstrates that the response may be dynamic and connected with the time needed to translate the mdm2 protein. The response takes place if the dissociation constant k between p53 and mdm2 varies from its normal value. Although it is widely believed that it is an increase in k that triggers the response, we show that the experimental behaviour is better described by a decrease in the dissociation constant. The response is quite robust upon changes in the parameters of the system, as required by any control mechanism, except for few weak points, which could be connected with the onset of cancer. Received 8 May 2002 / Received in final form 9 July 2002 Published online 17 September 2002     

Simulation of viscous water column collapse using adapting hierarchical grids

An adaptive hierarchical grid‐based method for predicting complex free surface flows is used to simulate collapse of a water column. Adapting quadtree grids are combined with a high‐resolution interface‐capturing approach and pressure‐based coupling of the Navier–Stokes equations. The Navier–Stokes flow solution scheme is verified for simulation of flow in a lid‐driven cavity at Re=1000. Two approaches to the coupling of the Navier–Stokes equations are investigated as are alternative face velocity and hanging node interpolations. Collapse of a water column as well as collapse of a water column and its subsequent interaction with an obstacle are simulated. The calculations are made on uniform and adapting quadtree grids, and the accuracy of the quadtree calculations is shown to be the same as those made on the equivalent uniform grids. Results are in excellent agreement with experimental and other numerical data. A sharp interface is maintained at the free surface. The new adapting quadtree‐based method achieves a considerable saving in the size of the computational grid and CPU time in comparison with calculations made on equivalent uniform grids. Copyright © 2005 John Wiley & Sons, Ltd.     

An AFM, XPS and electrochemical study of molecular electroactive monolayers formed by wet chemistry functionalization of H-terminated Si(1 0 0) with vinylferrocene

Molecular electroactive monolayers have been produced from vinylferrocene (VFC) via light-assisted surface anchoring to H-terminated n- and p-Si(1 0 0) wafers prepared via wet chemistry, in a controlled atmosphere. The resulting Si-C bound hybrids have been characterized by means of XPS and AFM. Their performance as semiconductor functionalized electrodes and their surface composition have been followed by combining electrochemical and XPS measurements on the same samples, before and after use in an electrochemical cell. White-light photoactivated anchoring at short (1 h) exposure times has resulted in a mild route, with a very limited impact on the initial quality of the silicon substrate. In fact, the functionalized Si surface results negligibly oxidized, and the C/Fe atomic ratio is close to the value expected for the pure molecular species. The VFC/Si hybrids can be described as (η⁵-C₅H₅)Fe²⁺(η⁵-C₅H₄)-CH₂-CH₂-Si species, on the basis of XPS results. Electrochemical methods have been applied in order to investigate the role played by a robust, covalent Si-C anchoring mode towards substrate-molecule electronic communication, a crucial issue for a perspective development of molecular electronics devices. The response found from cyclic voltammograms for p-Si(1 0 0) functionalized electrodes, run in the dark and under illumination, has shown that the electron transfer is not limited by the number of charge carriers, confirming the occurrence of electron transfer via the Si valence band. The hybrids have shown a noticeable electrochemical stability and reversibility under cyclic voltammetry (cv), and the trend in peak current intensity vs. the scan rate was linear. The molecule-Si bond is preserved even after thousands of voltammetric cycles, although the surface coverage, evaluated from cv and XPS, decreases in the same sequence. An increasingly larger surface concentration of Fe³⁺ at the expenses of Fe²⁺ redox centers has been found at increasing number of cv’s, experimentally associated with the growth of silicon oxide. Surface SiO⁻ groups from deprotonated silanol termination, induced by the electrochemical treatments, are proposed as the associated counterions for the Fe³⁺ species. They could be responsible for the observed decrease in the electron transfer rate constant with electrode ageing.     

Energy Spectrum Width and Nonequilibrium Energy of Rayleigh Waves Scattered on a Two-Dimensional Near-Surface Electron Layer

We obtain expressions for the energy spectrum widths of Rayleigh waves corresponding to their deformational coupling to Fermi and Boltzmann electrons in a two-dimensional layer near the surface of a semibounded solid. We evaluate the nonequilibrium energy of Rayleigh waves that depends on these widths and is caused by the same coupling to the corresponding hot electrons. We show that this energy is independent of the degeneracy degree of the electrons and is given by the mean energy of free Rayleigh waves heated up to temperature of the electrons. We find conditions under which the thermodynamics is determined by this nonequilibrium energy of Rayleigh waves in films of a certain thickness with Fermi electrons near the surface and by the equilibrium energy of bulk phonons in thicker samples. All the results are obtained using the Keldysh diagram technique applied to the case of semibounded media.