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     

用扫描隧道显微镜测量局域功函数

用扫描隧道显微镜在Cu（111）-Au和Pt（111）-Ag表面上对局域功函数进行了测量．在扫描的同时通过测量隧道电流对针尖样品间距离变化的响应，可以在得到扫描隧道显微镜（STM）图的同时得到功函数图．用这种方法，成功地观察到Au，Ag覆盖层与Cu，Pt衬底间的功函数的差别．结果表明：Au覆盖层的功函数介于Cu（111）和Au（111）的功函数之间，这与其它方法的结果一致．在Pt（111）-Ag表面观察到了局域功函数随覆盖层厚度的变化．本工作表明：扫描隧道显微镜在研究功函数与表面结构的关系方面是十分有用的；用测量局域功函数的方法还可以区分表面不同种的物质 关键词：     

面向燃料电池双极板的不锈钢表相掺杂耐蚀性高通量计算与分析

通过基于密度泛函理论(DFT)的第一性原理高通量计算,筛选了可以提高不锈钢双极板钝化层在PEMFCs工作环境中的耐蚀性的掺杂元素.基于Cr₂O₃的■切面构建计算模型,对其进行了48种元素的掺杂替换,考虑228种掺杂构型．根据掺杂结构和位移能量、掺杂元素被分为4类,并采用不同的吸附、空位计算方案．根据不同掺杂类型采用不同的吸附、空位计算方案,计算了每种掺杂元素对功函数、F的吸附能和Cr/O的空位形成能的影响.计算结果显示,C、N、In、Ru对于不锈钢钝化层的各项耐蚀性参数提升效果较好;Au、Rh、Pt、Ir、Co、Ni也能较好地提升耐蚀性,但是存在成本高或者危害质子膜的问题;Ag、Cu、Sn、Ge可以抑制空位形成和F吸附,但会造成功函数下降;Zn可以提高功函数并抑制F吸附.此外,对于电子态密度的计算表明,掺杂原子与Cr原子形成的稳定键合是耐蚀性参数提升的重要因素.     

三氧化钨表面氢吸附机理的第一性原理研究

采用基于密度泛函理论的第一性原理平面波超软赝势方法,在广义梯度近似下,研究了立方WO_3,WO_3(001)表面结构及其氢吸附机理.计算结果表明立方晶体WO_3理论带隙宽度为0.587 eV.WO_3(001)表面有WO终止(001)表面和O终止(001)表面两种结构,表面结构优化后W—O键长和W—O—W键角改变,从而实现表面弛豫;WO终止(001)表面和O终止(001)表面分别呈现n型半导体特征和p型半导体特征.分别计算了H原子吸附在WO终止(001)表面和O终止(001)表面的H—O_(2c)—H,H—O_(2c)…H—O_(2c),H—O_(1c)—H和H—O_(1c)…H—O_(1c)四种吸附构型,其中H—O_(1c)—H吸附构型的吸附能最小,H—O键最短,H失去电子数最多,分别为-3.684 eV,0.0968 nm和0.55e,此吸附构型最稳定.分析其吸附前后的态密度,带隙从吸附前的0.624 eV增加到1.004 eV,价带宽度基本不变.H的1s轨道电子与O的2p,2s轨道电子相互作用,在-8和-20 eV附近各形成了一个较强的孤立电子峰,两个H原子分别与一个O_(1c)原子形成化学键,最终吸附反应生成了一个H_2O分子,同时产生了一个表面氧空位.     

c(2×2)O吸附Cu(001)表面结构、电子态与STM图像的研究

用投影子缀加波和CP分子动力学方法研究了贵金属Cu(001)面的表面结构、弛豫以及O原子的c(2×2)吸附状态. 研究结果得出在这种吸附结构中，O原子与衬底Cu原子之间的垂 直距离约为0069nm，Cu—O键长为0.194nm，功函数约为5.29 eV；吸附O原子形成金属性能带结构，由于Cu—O的杂化作用,在费米能以下约6.7 eV处出现了局域的表面态.用Tersoff-Hamann途径计算了该表面的扫描隧道显微镜图像，并讨论了与实验结果之 间的关系. 关键词： Cu(001)-c(2×2)/O 电子态 STM图像     

外电场对NO在Graphene负载的Pd单原子上的吸附特性的调控

本研究中,通过基于密度泛函理论的第一性原理并考虑范德华力修正计算了Graphene负载的Pd单原子界面特性以及NO的吸附特性(包括吸附构型的结构参数、吸附能和电子结构等),并着重研究了电场对其吸附特性的调控规律及其内在机理.结果表明：1) NO在Pd/Graphene上能够形成较强的化学吸附,吸附能为1.09 eV.吸附的NO分子中的N-O键拉长. Pd-d态与NO-p态的强杂化作用都表明NO分子在Pd-Graphene上被活化. 2)在电场作用下Graphene负载的单原子Pd上的电荷随施加的电场逐渐变化. 3)跟没有施加电场的NO吸附的体系相比,当对NO吸附体系施加沿Z正方向的电场时,NO的吸附增加,吸附的NO从衬底获得更多的负电荷,而Pd所带的正电荷逐步减少;当对NO吸附体系施加沿Z负方向的电场时,NO的吸附减弱,吸附的NO从衬底获得的负电荷逐渐减少,而Pd所带的正电荷逐步增加. 4)外加电场能够有效地调控NO的吸附特性,并调控NO与衬底之间的电荷转移进而调控其电子结构.     

Fe_3O_4单晶薄膜磁性电场调控的微磁学仿真研究

磁性薄膜磁学特性电场调控的相关研究对开发新型低功耗磁信息器件具有突出意义.本文基于电场调控磁性的基本理论,以OOMMF(Object Oriented Micro-Magnetic Frame)微磁学仿真软件为工具,研究了电场对生长于PZN-PT单晶衬底上Fe_3O_4单晶薄膜磁学特性的调控.研究结果显示:无外加电场时,薄膜表现出典型的软磁特性;沿衬底[001]方向施加的外加电场可以使得薄膜矫顽力、矩形比等磁学特性发生显著改变:当外加磁场沿[100]([010])时,施加正值(负值)电场强度可以显著增大薄膜的矫顽力与矩形比,当电场强度不小于0.6 MV/m时薄膜矩形比达到1.这是因为外加电场导致薄膜产生单轴应力各向异性,使得薄膜的等效磁各向异性发生了从无外电场下的面内四重磁晶各向异性向高电场下的近似单轴磁各向异性的过渡.外加1 MV/m与-1 MV/m的电场时等效易磁化轴分别沿[100]与[010]方向.另外,外加1 MV/m(-1 MV/m)的电场强度可以使得铁磁共振的频率增大(减小)接近1 GHz.     

多重散射团簇理论对CO/NiO(100),NO/NiO(100)吸附系统的分析与比较

用多重散射团簇(MSC)理论对CO/NiO(100)和NO/NiO(100)吸附系统的C1s近边X射线吸收精细结构(NEXAFS)和N1sNEXAFS谱进行了详细的计算和分析.理论计算表明CO/NiO(100)是弱物理吸附,CO分子与表面的多极静电相互作用很弱,σ共振不依赖C—O键长的变化,MSC方法分析表明,CO是以C原子朝下,吸附在衬底的Ni—O键桥上,可靠性因子计算显示C原子的吸附位置距Ni原子009nm,CO分子中C原子距衬底的吸附高度为031±001nm,CO分子倾斜角不大于25°.理论计算证实     

金属/石墨烯复合纳米阵列结构LSPR特性

利用离散偶极近似(Discrete Dipole Approximation,DDA)方法系统研究金属/石墨烯复合纳米阵列的消光特性,考察金属基底和石墨烯纳米阵列尺寸对局域表面等离子体共振峰位和强度的影响,以及研究不同基底厚度比条件下纳米复合阵列的电场分布、规律和物理本质。仿真结果表明,当保持金属基底厚度不变时,Ag/Au/石墨烯复合纳米阵列的局域表面等离子体共振峰随石墨烯原子层数的增大而增大,共振波长发生微小红移;当保持八根石墨烯层柱和银基底厚度不变时,随金银厚度比的增大,消光光谱发生蓝移;Ag/Au/石墨烯复合纳米阵列银层表面的电场强度为最强,石墨烯纳米棒阵列的电场强度较强。     

电场作用下P掺杂硅烯选择性吸附CH_4的第一性原理计算

在煤层气中选择性吸附和捕捉甲烷分子,对提高煤矿安全具有十分重要的意义.本文采用第一性原理计算的方法,研究了外加电场作用下P掺杂硅烯对甲烷分子的选择性吸附性能.结果表明:正电场作用下,P掺杂硅烯与甲烷分子之间产生较强的化学吸附,能够快速捕获甲烷分子.当关闭外加电场时,P掺杂硅烯与甲烷分子之间则为微弱的物理吸附,甲烷分子很容易实现脱附.同时还发现,外加电场作用下,P掺杂硅烯与氮气、氧气及水之间的吸附均属于物理吸附,表明P掺杂硅烯可以在这些混合气体中实现甲烷气体的选择性吸附. P掺杂硅烯有望成为选择性好的甲烷传感、捕获新材料.     

Collective modes,damping, and the scattering function in classical liquids

An exact representation for the density-density response function is presented. This representation is a generalization of the result obtained in the mean field approximation and amounts to replacing the static, effective potential by one which is both wavenumber- and frequency-dependent. This potential possesses both a real and an imaginary part; the latter describes the collisional damping of collective modes. Analyticity and sum rule arguments are used to describe the basic properties of this complex potential. The formalism allows us to write an exact formula for the scattering functionS(k, ) in which the basic unknown is the collisional damping function. Using a small portion of the recent experimental data on coherent neutron scattering in liquid argon, we are able to calculateS(k, ) and other quantities of interest and to make comparisons with the rest of the data.     

Excitation function of (p, pn) reactions at high energy

A closed theoretical formula for the (p, pn) reaction cross section at high energies in light, medium and heavy nuclei has been derived, and a comparison of the calculated cross sections with the experimental datais made for ¹²C, ¹⁹F, ⁵⁴Fe, ⁵⁸Ni, ⁵⁹Co, ⁶⁴Zn, ⁶⁵Cu, ¹⁰⁰Mo, ¹²⁷I, ¹⁴²Ce, ¹⁸²Ta and ²³⁸U at incident energies above 50 MeV. Good agreement between experimental and calculated cross sections is obtained in the entire energy range considered. In deducing the formula a direct reaction with a pure knock-out mechanism has been assumed.     

热超构材料：几何结构、工作机制与新奇性质

因为在热保护、热探测和热管理领域存在重要的应用价值,自由操控宏观热流一直是人类的 一个梦想。热超构材料正是为此目的应运而生,它是电磁超构材料在热学领域的延伸。在此,我将 综述该领域自2008 年诞生以来取得的若干研究进展,其将主要包括以下新奇热现象或功能器件： 热隐身;热聚集;热旋转;宏观热二极管;热伪装;热透明;热晶体;环境温差中零能耗保温;宏 观热网络中反常热传导;热对流隐身、聚集、伪装;热辐射制冷。我将介绍与之相关的微观或宏观 传热机制,这些机制可以通过以下理论或方法来理解或阐述：变换热学理论、Laplace 方程、热声 子能带理论、相变理论、变换热对流理论、热辐射制冷理论。我也将介绍这些材料从基础研究到工 业应用的发展前景。     

Nucleon/nuclei polarized structure function,using Jacobi polynomials expansion

We use the constituent quark model to extract polarized parton distributions and finally polarized nucleon structure function.Due to limited experimental data which do not cover whole （x,Q 2 ） plane and to increase the reliability of the fitting,we employ the Jacobi orthogonal polynomials expansion.It will be possible to extract the polarized structure functions for Helium,using the convolution of the nucleon polarized structure functions with the light cone moment distribution.The results are in good agreement with available experimental data and some theoretical models.     

Freezing transition, characteristic polynomials of random matrices, and the Riemann zeta function

We argue that the freezing transition scenario, previously explored in the statistical mechanics of 1/f-noise random energy models, also determines the value distribution of the maximum of the modulus of the characteristic polynomials of large N×N random unitary matrices. We postulate that our results extend to the extreme values taken by the Riemann zeta function ζ(s) over sections of the critical line s=1/2+it of constant length and present the results of numerical computations in support. Our main purpose is to draw attention to possible connections between the statistical mechanics of random energy landscapes, random-matrix theory, and the theory of the Riemann zeta function.     

Work function changes and surface chemistry of oxygen, hydrogen, and carbon on indium tin oxide

The surface chemistry of indium tin oxide (ITO) has been investigated with Auger electron spectroscopy (AES) and high resolution electron energy loss spectroscopy (HREELS). A vibrating Kelvin probe (KP) with a graphite reference was used to monitor the absolute work function (Φ) of ITO as a function of chemical modification. The ITO was exposed in situ to molecular hydrogen (H₂), hot-filament-activated oxygen (O₂^*), and hot-filament-activated deuterium (D₂^*). The initial Φ of ITO was determined to be 5.2 eV, and surface chemical changes had strong effects on this value, as seen by KP. Exposure of clean ITO to O₂^* increased Φ to 5.6 eV, but the increase was short-lived. The changes in Φ over time were correlated with the uptake of carbon impurities in ultra high vacuum (UHV), as monitored by AES.

The HREELS of ITO revealed significant hydrocarbon impurities. Chemical reduction of ITO produced a metallic surface and dehydrogenated the adsorbed hydrocarbons. Both re-oxidation of metallic ITO and oxidation of clean ITO temporarily removed adventitious carbon from the surface, but oxidized ITO adsorbed an even larger quantity of carbon over time.     

Modeling, measuring, and minimizing the instrument response function of a tunable diode laser spectrometer

The instrument response function (IRF) of a spectrometer limits the accuracy of measured spectroscopic parameters by broadening recorded spectral lines/features. We describe methods to model the effects of the IRF on spectral data, to minimize the IRF widths, and to measure the resulting width of the spectrometer IRF. We have modeled the IRF of our Tunable Diode Laser Spectrometer as a Voigt function. A real-time method of eliminating the effects of low-frequency spectrometer drift has been implemented and has resulted in a substantial reduction in the width of the IRF, its residual Gaussian component reduced from about to about . An accurate measurement of the IRF Gaussian width utilizes a computationally simple method making use of the spectral dependence of the RMS noise of each signal-averaged data point. Various noise sources affecting the spectrometer (preamp/detector noise, laser AM noise, and laser FM noise) are identified and separately quantified by use of the same method. The IRF Gaussian-width measurement can be automatically applied to each measured spectrum of an experimental data set. A related method is discussed which allows accurate determination of the spectral dependence of statistical noise appropriate for use in quantitative Chi-square fitting of absorption spectra. We explore simple, efficient numerical processes which can dramatically enhance the quality and usefulness of acquired spectral data, improving the ability to apply TDL spectroscopy to high-precision, quantitative measurements and the determination of detailed spectroscopic lineshape parameters. This paper provides a guide for interested readers to implement these developments in their own spectrometers.     

谱相关的原理、功能与α截面谱表示

讨论了Gardner原始文献未论述的谱相关的数学起源与物理功能问题.指出谱相关的物理功能为一个广义2倍频与自混频器.讨论了信号谱相关的优势与局限.给出了Gardner原始文献所遗漏的循环频率α截面的谱相关表示.给出了无线电信号谱相关物理功能的计算实例 关键词： 谱相关 可调和 循环平稳过程的自相关 物理功能     

GLM equations,tau function and scattering data

The direct and the inverse scattering problem for affine Toda/mKdV systems is addressed and is found to develop non-standard features within the framework of the inverse scattering method. A solution scheme based on the tau function formalism is described. The inverse problem is shown to be equivalent to a set of decoupled, scalar Gelfand-Levitan-Marchenko-type equations. The Fredholm-Grothendieck determinants of the latter are shown to define tau-functions in the sense of the Kyoto School. In particular, a simple monodromy formula allows the derivation of trace identities.     

Black hole entropy function,attractors and precision counting of microstates

In these lecture notes we describe recent progress in our understanding of attractor mechanism and entropy of extremal black holes based on the entropy function formalism. We also describe precise computation of the microscopic degeneracy of a class of quarter BPS dyons in supersymmetric string theories, and compare the statistical entropy of these dyons, expanded in inverse powers of electric and magnetic charges, with a similar expansion of the corresponding black hole entropy. This comparison is extended to include the contribution to the entropy from multi-centred black holes as well.