Cs/GaN(0001)吸附体系电子结构和光学性质研究

采用基于第一性原理的密度泛函理论平面波超软赝势方法计算了 1/4ML Cs原子吸附 (2 × 2) GaN(0001) 表面的吸附能、能带结构、电子态密度、电荷布居数、功函数和光学性质. 计算发现, 1/4ML Cs 原子在 GaN(0001) 表面最稳定吸附位为 N 桥位, 吸附后表面仍呈现为金属导电特性, Cs原子吸附GaN(0001)表面后主要与表面 Ga 原子发生作用, Cs6s 态电子向最表面 Ga 原子转移, 引起表面功函数下降. 研究光学性质发现, Cs 原子吸附 GaN(0001) 表面后, 介电函数虚部、吸收谱、反射谱向低能方向移动.     

Electrodynamics of spin currents in superconductors

In recent work we formulated a new set of electrodynamic equations for superconductors as an alternative to the conventional London equations, compatible with the prediction of the theory of hole superconductivity that superconductors expel negative charge from the interior towards the surface. Charge expulsion results in a macroscopically inhomogeneous charge distribution and an electric field in the interior, and because of this a spin current is expected to exist. Furthermore, we have recently shown that a dynamical explanation of the Meissner effect in superconductors leads to the prediction that a spontaneous spin current exists near the surface of superconductors (spin Meissner effect). In this paper we extend the electrodynamic equations proposed earlier for the charge density and charge current to describe also the space and time dependence of the spin density and spin current. This allows us to determine the magnitude of the expelled negative charge and interior electric field as well as of the spin current in terms of other measurable properties of superconductors. We also provide a `geometric' interpretation of the difference between type I and type II superconductors, discuss how superconductors manage to conserve angular momentum, discuss the relationship between our model and Slater's seminal work on superconductivity, and discuss the magnitude of the expected novel effects for elemental and other superconductors.     

Covalent functionalization of AlN nanotubes with acetylene

Covalent functionalization of a zigzag AlN nanotube (AlNNT) with acetylene molecule has been investigated using density functional theory in terms of energetic, geometry and electronic properties. The obtained results show that the acetylene preferably tends to [2+2] addition on Al–N bonds of the tube surface releasing energies in the range of 1.02 to 1.10 eV along with a charge transfer from the tube to the acetylene. We have found that HOMO–LUMO gap of AlNNT has not changed significantly upon the functionalization and, its global hardness and electrophilicity are slightly decreased. Also, it has been revealed that the field electron emission from the AlNNT surface may be improved upon the adsorption of acetylene due to decrease of work function ascribed to the charge transfer from the tube to the acetylene.     

氧在Nb(110)表面吸附的第一性原理研究

通过第一性原理赝势平面波方法研究了氧在Nb(110)表面的吸附性质随覆盖度变化规律. O在Nb(110)表面最稳定吸附位是洞位,次稳定吸附位是长桥位. 在长桥位吸附时, O诱导Nb(110)表面功函数随覆盖度的增加而几乎线性增加;但当O在洞位吸附时, 与干净Nb表面相比, 覆盖度为0.75 ML和1.0 ML时功函数增加, 而覆盖度为0.25 ML和0.5 ML时功函数减小.通过对面平均电荷密度分布和偶极矩变化的讨论, 解释了由吸附导致功函数复杂变化的原因.通过对表面原子结构和态密度分析, 讨论了O在Nb表面吸附时引起表面原子结构变化以及O和Nb(110)表面原子的相互作用.     

The surface potential of insulating thin films negatively charged by a low-energy focused electron beam

We report on the surface potential characteristics in the equilibrium state of the grounded insulating thin films of several 100 nm thickness negatively charged by a low-energy (<5 keV) focused electron beam, which have been simulated with a newly developed two-dimensional self-consistent model incorporating electron scattering, charge transport and charge trapping. The obtained space charge is positive and negative within and outside the region, respectively, where the electron and hole densities are greater than the trap density. Thus, the surface potential is relatively high around the center, then it decreases to a maximum negative value and finally tends to zero along the radial direction. The position of the maximum value is far beyond the range of e-beam irradiation as a consequence of electron scattering and charge transport. Moreover, a positive electric field can be generated near the surface in both radial and axial directions. The surface potential at center exhibits a maximum negative value in the condition of the ～2 keV energy non-penetrating e-beam in this work, which is supported by some existing experimental data in scanning electron microscopy. Furthermore, the surface potential decreases with the increase in beam current, trap density and film thickness, but with the decrease in electron mobility.     

Surface charge carrier motion on insulating surfaces: One dimensional motion

We consider a model for the motion of charge carriers on the surface of an insulator. The insulator surface is either infinite, semi–infinite against a conducting half space or a strip between two conducting half spaces. The charge flux on the surface is assumed equal to the charge density times the electric field component in the surface, with time a constant. When the charge carrier motion in the plane is assumed constant in one direction, we can write the problem as an inviscid Burgers equation for a complex function. The imaginary part of this function is minus the carrier density while the real part, the Hilbert transform of the carrier density, is minus the electric field on the surface. Using the method of characteristics, we find an exact implicit solution for the problem and illustrate it with several examples. One set of examples, on the real line, or half of it, show how charge moves and how the surface may discharge into a conducting wall. They also show that the system can sustain shock wave solutions which are different from those in a real Burgers equation and other singular behaviour. Exact solutions on a finite strip between two conducting walls also show how that system can discharge completely, and also demonstrate shock waves. These systems are of particular interest because they are experimentally accessible.     

Universal fermionic spectral functions from string theory

We carry out the first holographic calculation of a fermionic response function for a strongly coupled d=3 system with an explicit D=10 or D=11 supergravity dual. By considering the supersymmetry current, we obtain a universal result applicable to all d=3 N=2 SCFTs with such duals. Surprisingly, the spectral function does not exhibit a Fermi surface, despite the fact that the system is at finite charge density. We show that it has a phonino pole and at low frequencies there is a depletion of spectral weight with a power-law scaling which is governed by a locally quantum critical point.     

Electronic structure of K-(001) surface by the density matrix method

The electronic structure of the (001) surface of b.c.c. K has been studied by a direct determination of the density matrix in a local orbital basis. The method is based on a variational treatment of the ground state energy applying the Hohenberg-Kohn-Sham functional formalism. Surface charge density, work function and surface energy are in good agreement with other first principle self consistent calculations.     

电介质/半导体结构样品电子束感生电流瞬态特性

电子束照射下电介质/半导体样品的电子束感生电流(electron beam induced current,EBIC)是其电子显微检测的重要手段.结合数值模拟和实验测量,研究了高能电子束辐照下SiO2/Si薄膜的瞬态EBIC特性.基于Rutherford模型和快二次电子模型研究电子的散射过程,基于电流连续性方程计算电荷的输运、俘获和复合过程,获得了电荷分布、EBIC和透射电流瞬态特性以及束能和束流对它们的影响.结果表明,由于电子散射效应,自由电子密度沿入射方向逐渐减小.由于二次电子出射,净电荷密度呈现近表面为正、内部为负的特性,空间电场在表面附近为正而在样品内部为负,导致一些电子输运到基底以及一些出射二次电子返回表面.SiO2与Si界面处俘获电子导致界面附近负电荷密度高于周围区域.随电子束照射样品内部净电荷密度逐渐降低,带电强度减弱.同时,负电荷逐渐向基底输运,EBIC和样品电流逐渐增大,电场强度逐渐减小.由于样品带电强度较弱,表面出射电流和透射电流随照射基本保持恒定.EBIC、透射电流及表面出射电流均随束流呈现近似正比例关系.对于本文SiO2/Si薄膜,透射电流随束能的升高逐渐增大并接近于束流值,EBIC在束能约15 keV时呈现极大值.     

Emission and accretion of electrons by negatively charged dust particles in a plasma

Taking into account the image force on the electron and Debye shielding an expression for the reduction in the work function for a spherical metallic particle in a dusty plasma on account of the negative charge on the surface has been derived. The dependence of the reduction of the work function on the charge on the particle and Debye radius has been tabulated. The effect of this reduction on the thermionic and photoelectric emission and accretion of electrons by the particle has been discussed. As an interesting application of the work, the observed enhancement of the photoelectric emission from individual micron size grains with increasingly negative surface potential has been explained; the grains were selected from samples of dust collected in the Apollo-17 and Luna-24 missions.     

Interaction of bathocuproine with metals (Ca, Mg, Al, Ag, and Au) studied by density functional theory

Electronic structure of the interface between a bathocuproine (BCP) molecule and metal surface was studied by density functional theory. The bond energy of BCP with metal surface increased with decreasing work function of metals, that is, Au, Ag, Al, Mg, and Ca in this order. The charge transfer also increased with decreasing metal work function. It was analyzed that the Fermi level and the lowest unoccupied molecular orbital of BCP are composed of both BCP and metal orbital component, and electron transport properties across the BCP and metal is discussed based on these analyses.     

Surface phase transition in H/W(110) induced by tuning the fermi surface nesting vector by hydrogen loading

At a hydrogen coverage of one monolayer, W(110) is known to exhibit a Fermi nesting in its electronic surface states with a nesting vector q{N} of 0.9 A{-1} along [001]. Here we show that additional H adsorption allows a controlled tuning of q{N}. As q{N} approaches the commensurate value of 1.0 A{-1}, its signature in inelastic He-atom scattering becomes more pronounced, finally disappearing as a surface charge density wave (CDW) develops and the surface symmetry changes from c(2 x 2) to a p(8 x 2) superstructure. The gradual change in q{N} is attributed to an energetic shift of the spin-polarized electronic surface states that eventually form the surface CDW.     

Changes in work function due to charge transfer in chemisorbed layers

In a simple tight-binding model well suited to transition and noble metals, we calculate the work function change due to adsorption of alkali metals. A decrease is found to be caused by ionic bonds formed on the surface through charge transfer between the two metals. The local density of states and the number of electrons in the substrate and the chcmisorbed layer are evaluated for various alkali metals and coverages. The method is applicable in both the high and low coverage limits in contrast to existing theories.     

第一性原理计算Ni原子吸附在Al(111)表面原子结构和电子态

利用密度泛函理论和广义梯度近似研究镍吸附在Al(111)表面。在覆盖率为0.25ML下,分析了Ni吸附在Al(111)表面的面心立方洞位、六角密排洞位、顶位和桥位四个高对称位的原子结构和吸附能。比较不同高对称位的吸附能发现,六角密排洞位的吸附能最大,是5.76 eV,是最稳定的吸附位置。详细讨论了两个最低能量结构-三重洞位的电子结构、功函数、表面偶极距和Ni-Al键的特性。在费米能级附近,Ni-3d和Al-3s,3p轨道产生杂化,形成金属间化合键。由于吸附导致双金属体系表面偶极距和功函数的变化。我们发现：Ni原子与Al(111)表面原子间成建主要是共价键,没有表现出明显的静电荷跃迁,相应的产生非常小的表面偶极距。与面心立方洞位相比,六角密排洞位在费米能级附近产生较低的态密度,在键态附近产生较大的杂化。     

Methane adsorption on graphite（0001） films： A first-principles study

Using first-principles methods, we have systematically investigated the electronic density of states, work function, and adsorption energy of the methane molecule adsorbed on graphite(0001) films. The surface energy and the interlayer relaxation of the clean graphite(0001) as a function of the thickness of the film were also studied. The results show that the interlayer relaxation is small due to the weak interaction between the neighboring layers. The one-fold top site is found most favourable on substrate for methane with the adsorption energy of 133 meV. For the adsorption with different adsorption heights above the graphite film with four layers, the methane is found to prefer to appear at about 3.21 A above the graphite. We also noted that the adsorption energy does not dependent much on the thickness of the graphite films. The work function is enhanced slightly by adsorption of methane due to the slight charge transfer from the graphite surface to the methane molecule.     

Variations of work function and surface conductivity on clean cleaved zinc oxide surfaces by annealing and by hydrogen adsorption

Crystals are cleaved in UHV normal and parallel to the c axis exposing polar and prism faces. Work function (Kelvin) and surface conductivity are measured, also after annealing at elevated temperatures in UHV and after adsorption of atomic hydrogen. The work function of all three faces decreases irreversibly by annealing in UHV, but only on the Zn face a measurable surface conductivity appears. Also hydrogen adsorption diminuishes the work function. Simultaneously an increasing surface conductivity can be observed on all three types of surfaces. Corresponding structures in the annealing curves demonstrate a correlation between work function and surface conductivity. By means of space charge calculations band bending values are derived and there-by the electron affinity, which is not accessible to direct measurement. It is concluded that the two clean cleaved polar faces exhibit a depletion layer, which remains on the O face also after annealing in UHV. On the prism face nearly flat band situation is found. The decrease of work function with increasing hydrogen coverage, i.e. surface electron density, can be interpreted by means of space charge calculations using the measured surface conductivity. For the two polar faces the band bending alone causes the decrease, whereas for the prism face an additional increase of electron affinity has to be assumed. The variation of electron affinity by annealing or by hydrogen adsorption might be due to a change of atomic distances in the uppermost layer, although no superstructure has been found in LEED studies.     

盐离子对蛋白质带电特性的影响

本文应用分子理论,研究盐离子对蛋白质带电特性的影响,理论模型考虑蛋白质与阴离子的结合作用。研究发现,由于蛋白质与阴离子的结合,距离蛋白质表面附近处的阴离子被吸附在了蛋白质表面,在距离蛋白质表面附近区域,阴离子分布较少。通过计算体系中的静电势,我们发现,在距离蛋白质表面附近,静电势呈现了较大的负值,带正电荷的阳离子感受到静电吸引,会出现在距离蛋白质表面附近的区域,这会使得在距离蛋白质表面附近的区域,阳离子数目增多。这样,在不同阴离子浓度、以及阴离子与蛋白质不同结合能条件下,阴离子会在不同程度上影响蛋白质的带电特性、影响体系中的静电特性。通过考察不同结合能条件下,蛋白质表面电荷面密度随阴离子浓度的变化关系还发现,较大的结合能会使得阴离子与蛋白质结合增快,蛋白质表面会呈现从正电荷态向负电荷态的转变。理论结果符合实验观测,由此表明,盐离子与蛋白质的结合导致蛋白质表面带电特性的改变,是盐离子影响蛋白质带电特性的本质。     

Self-consistent pseudopotential calculation for the (111) surface of aluminum

The electronic structure of the (111) surface of aluminum is calculated using self-consistent pseudopotentials. Surface states are identified and the (111) work function calculated. The behavior of the total charge density and potential near the surface is displayed and discussed. Self-consistency is found to be of crucial importance.     

Performance of the constrained minimization of the total energy in density functional approximations: the electron repulsion density and potential

In the constrained minimization method of Gidopoulos and Lathiotakis [N.I. Gidopoulos, N.N. Lathiotakis, J. Chem. Phys. 136, 224109 (2012)], the Hartree exchange and correlation Kohn-Sham potential of a finite N-electron system is replaced by the electrostatic potential of an effective charge density that is everywhere positive and integrates to a charge of N ? 1 electrons. The optimal effective charge density (electron repulsion density, ρ_rep) and the corresponding optimal effective potential (electron repulsion potential v_rep) are obtained by minimizing the electronic total energy in any density functional approximation. The two constraints are sufficient to remove the self-interaction errors from v_rep, correcting its asymptotic behavior at large distances from the system. In the present work, we describe, in complete detail, the constrained minimization method, including recent refinements. We also assess its performance in removing the self-interaction errors for three popular density functional approximations, namely LDA, PBE and B3LYP, by comparing the obtained ionization energies to their experimental values for an extended set of molecules. We show that the results of the constrained minimizations are almost independent of the specific approximation with average percentage errors 15%, 14%, 13% for the above DFAs respectively. These errors are substantially smaller than the corresponding errors of the plain (unconstrained) Kohn-Sham calculations at 38%, 39% and 27% respectively. Finally, we showed that this method correctly predicts negative values for the HOMO energies of several anions.