分子动力学模拟Gd原子在Cu(110)表面的扩散过程

为了分析Gd吸附原子在Cu(110)表面的扩散机理，用分子动力学对该扩散过程进行模拟.模拟 结果表明在［1 1 0］方向Gd原子通过跳跃机理扩散，而且多步跳跃频率很高.而在［0 0 1］方向则通过交换机理扩散.吸附原子在［1 1 0］方向的扩散能力要比［0 0 1］ 方向强.通过对扩散频率的拟合，发现两种扩散机理都符合Arrhenius公式，从而确定了跳跃 机理的扩散势垒为0.097eV，交换机理的扩散势垒为0.33eV.另外还用能量弛豫的方法确定了 跳跃机理的扩散势垒. 关键词： 分子动力学 表面扩散 跳跃机理 交换机理 扩散势垒     

Cu(111)三维表面岛对表面原子扩散影响的分子动力学研究

采用嵌入原子方法的原子间相互作用势，利用分子动力学方法计算了同质外延生长中不同层数的三维Cu(111)表面岛上表面原子扩散激活能，分析了三维表面岛的层数对表面原子交换扩散和跳跃扩散势垒的影响. 研究结果表明，二维Enrilich-Schwoebel(ES)势垒小于三维ES势垒，且三维ES势垒不随表面岛层数的增加而显著变化. 对于侧向表面为(100)的表面岛，表面原子沿〈011〉方向上的扩散行为，随表面岛层数增加而逐渐变化；在表面岛层数达到3层时，扩散路径上的势垒变化趋于稳定，表面原子扩散以下坡扩散为主. 对于侧面取向为(111)的表面岛，当表面岛层数大于3层后，开始呈现上坡扩散的可能. 关键词： 表面原子 扩散 分子动力学模拟     

氧原子在Pt(111)表面和次表层的吸附与扩散

氧原子在Pt表面的吸附和扩散是理解氧化和腐蚀等问题的基础.基于密度泛函理论和周期平板模型研究了氧原子在Pt(111)表面及次表层的吸附,通过扫描隧道显微镜(STM)的理论计算分析了吸附的结构特征.采用CI-NEB方法讨论了氧原子在Pt(111)表面和次表层的扩散过程.研究结果表明氧原子在Pt(111)表面的扩散比较容易,而氧原子向次表层的扩散相对较难,这主要是因为次表层的扩散需要经过一个Pt原子层,必须克服一定的能垒,从而说明过渡金属Pt具有很强的抗氧化性.     

电场下用扫描隧道显微镜对针尖原子扩散的观察

用扫描隧道显微镜（STM）研究了在金针尖和金样品间施加大偏压时所发生的各种不同的现象．在缓变大偏压的作用下，观察到针尖原子会发生场致扩散，导致针尖形状发生变化，并且还观察到了场发射和共振隧穿现象．提出了针尖原子的场致扩散是偏压电场使针尖表面极化引起的这一机理，并且指出了这种场致扩散在用大脉冲偏压作表面加工中起着重要的作用 关键词：     

研究单原子分子表面扩散运动的时域隧穿电流谱方法

以单个Cu原子在Si(111)(7×7)层错半单元(FHUC)内的随机扩散运动研究为例,演示了一种新的可以测量快速扩散运动的扫描隧道显微镜方法──时域隧穿电流谱方法.运用这种方法可定量地检测纳米局域区间内单原子分子的表面扩散运动,跳跃频率的测量范围达到1—104Hz,比过去已有的用扫描隧道显微镜研究表面扩散的方法提高三个量级.这种方法将会使人们在原子尺度下对快速扩散运动比如氢原子的量子扩散运动获得更进一步的理解.     

表面Cu原子间相互作用对Cu(001)表面跳跃扩散行为的影响

采用嵌入原子方法的原子间相互作用势，利用准静态分子动力学模拟研究了Cu原子在Cu(001)表面吸附所导致的基体晶格畸变以及对其附近的另一个吸附原子自扩散行为的影响.研究结果表明，吸附原子的存在可以导致多达10层的Cu基体晶格产生畸变.两个吸附原子所产生的晶格畸变应力场之间的相互作用，可以导致吸附原子运动活性的增加.通过比较同一路径上往返跳跃扩散势垒的差异发现，在原子间相互作用势的有效距离之外，两个吸附原子的扩散行为可以认为是存在晶格畸变应力场相互作用的两个独立吸附原子的扩散；在原子间相互作用势的有效距离之 关键词： 表面吸附原子 晶格畸变 表面二聚体 扩散     

钴原子及其团簇在Rh(111)和Pd(111)表面的扫描隧道显微学研究

利用扫描隧道显微镜和扫描隧道谱(STM/STS)及单原子操纵,系统研究了单个钴原子(Co) 及其团簇在Rh (111)和Pd (111)两种表面的吸附和自旋电子输运性质. 发现单个Co原子在Rh (111)上有两种不同的稳定吸附位,分别对应于hcp和fcc空位, 他们的高度明显不同,在针尖的操纵下单个Co原子可以在两种吸附位之间相互转化. 在这两种吸附位的单个Co原子的STS谱的费米面附近都存在很显著的峰形结构, 经分析认为Rh (111)表面单个Co原子处于混价区,因此这一峰结构是d轨道共振 和近藤共振共同作用的结果.对于Rh (111)表面上的Co原子二聚体和三聚体, 其费米面附近没有观测到显著的峰,这可能是由于原子间磁交换相互作用 和原子间轨道杂化引起的体系态密度改变所共同导致.与Rh (111)表面不同, 在Pd (111)表面吸附的单个Co原子则表现出均一的高度.并且对于Pd (111)表面所有 单个Co原子及其二聚体和三聚体,在其STS谱的费米面附近均未探测到显著的电子结构, 表明Co原子吸附于Pd (111)表面具有与Rh (111)表面上不同的原子-衬底相互作用与自旋电子输运性质.     

扫描隧道显微镜功能化针尖对分子能级的选择成像

文章提出了一种通过修饰STM针尖使其功能化，调节扫描隧道显微镜（STM）的扫描偏压范围，实现对分子能级的选择性成像的方法．二萘嵌苯分子在Ag（110）表面上自组织形成的有序单层膜主要是通过分子的π电子态成像，而被二萘嵌苯分子修饰的STM针尖的能级失配于基底上吸附的分子的能级，从而只对分子的部分能级成像．这个结果为有机界面电子输运测量提供了一种更好的能级选择方法．     

Ge(112)-(4×1)-In表面重构的原子结构

用扫描隧道显微镜(STM)研究了亚单层In原子引起的Ge(112)-(4×1)-In表面重构.结合随偏压极性不同而显著不同的STM图象和相应的“原子图象”,为这个重构提出了一个原子结构模型,供进一步研究参考.其中,In原子的吸附位置与它在Si(112)表面的吸附位置一致,但与Al原子和Ga原子在Si(112)表面的吸附位置不同.这个吸附位置的不同主要是由In原子较长的共价键键长引起的 关键词： 表面结构 In Ge 扫描隧道显微镜(STM)     

石墨单晶表面原子的扫描隧道显微象

扫描隧道显微镜(STM)是近几年发展起来的一种直接观察物质表面微观结构的仪器.利用量子隧道效应,将极细的金属针尖接近样品表面扫描,从而获得样品表面的三维图象,可以反映表面原子排列和原子形态.图1是我们设计制造的扫描隧道显微镜原理图.采用压电陶瓷管P作为x,y和z方向的三维扫描器件.管表面等分为相邻90°的四个电极,针尖T固定在其中的一个电极上.尖端曲率半径为100nm左右的金属针尖,可用化学腐蚀法制备.两对电极上施加扫描电压时,针尖便在垂直于管轴z的x-y方向扫描,而z方向的高低变化则由加在内管壁上的电     

Diffusive atom transport along step edges on Ag(1 1 1) at 295 K

The entropy-driven relaxation of a unique, non-equilibrium step edge configuration on the Ag(1 1 1) surface was observed using time-resolved STM imaging at room temperature. Using the Gibbs–Thomson relation, the relaxation process is quantitatively described as diffusive mass transport in terms of a gradient in the chemical potential along the monoatomic step edge. The STM data directly show that mass transport on Ag(1 1 1) is dominated by step edge diffusion at 295 K, and allow an estimate of the corresponding effective energy barrier. We obtain E_eff=0.49±0.05 eV and compare this value with recent results on island diffusion studies.     

Atomic diffusion inside a STM junction: simulations by kinetic Monte Carlo coupled to tunneling current calculations

The influence of a static scanning tunneling microscope (STM) tip on the diffusion of xenon atoms adsorbed on a Cu(1 1 0) stepped surface is studied. Semi-empirical potentials for the Xe-surface interaction and a N-body energy based method for the Xe-tip contribution are used to calculate the adsorption energy of adsorbates in the STM junction. First, we analyse the variation of this energy when the adatom is placed near a step edge and for different tip positions. When the tip is situated in the neighbourhood of the step edge, the Ehrlich-Schwoebel barrier experienced by the adatom is lowered. This opens a specific diffusion channel, allowing a possible crossing of the step edge. Second, through a kinetic Monte Carlo approach coupled to the elastic scattering quantum chemistry method, the noisy tunneling current created by the random motion of diffusing atoms in the vicinity of the tip can be analyzed. We show that, by counting the number of diffusion events, we can determine effective barriers related to the most dominant processes contributing to the diffusion at a particular temperature. We also demonstrate that the interaction mode of the tip (attractive or imaging) greatly modifies the diffusion processes.     

Smoothing of an atomically rough vicinal surface – STM observation and MC simulation

Smoothing of an atomically rough vicinal surface of SrTiO₃ is studied by scanning tunneling microscope (STM) observation and by Monte Carlo (MC) simulation. A complex step pattern that resembles a two-dimensional phase separation pattern is observed on the surface. Analysis of the step pattern during annealing obtained by the STM in comparison with the MC simulation reveals an asymmetry of the relaxation pattern between islands and holes. The asymmetry is attributed to the difference of the mobility of an adatom and an atomic hole, and the asymmetry is enhanced by the step edge diffusion barrier. Values of an effective bond energy and an effective diffusion barrier as well as the surface diffusion coefficient are deduced from the relaxation pattern.     

Fast dimer diffusion near the island: A computational study

Performing atomic scale simulations, we study the diffusion of small Co clusters on Cu(111) surface in the presence of Co islands. It is revealed that mesoscopic relaxations at the island-substrate interface play an important role during the diffusion events of the clusters. The diffusion barrier of small Co clusters near the islands increases with increasing cluster size. Especially, we find that dimer diffusion near the island with B step is as fast as monomer’s, which might be responsible for the formation of dendritic shaped islands at low temperature.     

STM imaging of electrically floating islands

Appearances and disappearances of Gd islands grown on top of a W(1 1 0) substrate were observed in time scales of hours after exposing the surface to a few Langmuirs of hydrogen. The phenomenon is presented and explained in terms of (temporary) creation of electrically floating islands, due to electrical decoupling of the island and substrate by the hydrogen that diffuses into the island/substrate interface. The disappearance of such an island is explained by forming a double barrier junction consisting of two tunneling barriers in series, causing, by charging, the potential of the island to become equal to that of the tip. The island then becomes “invisible” and the tip follows the corrugation of the surface under the substrate. The reappearance follows hydrogen mobility that retains the electrical conductivity of the island-substrate interface.     

MANIPULATION OF ATOMS, MOLECULES AND CLUSTERS FOR CONSTRUCTION OF NANOSYSTEMS

Controlled manipulations with the scanning tunneling microscope (STM) down to the scale of small molecules and single atoms allow to built molecular and atomic nanosystems, leading to the fascinating possibility of creating manmade structures on atomic scale. Here we present a short review on atomic scale manipulation investigations. Upon soft lateral manipulation of adsorbed species, in which only tip/particle forces are used, three different manipulation modes (pushing, pulling, sliding) can be discerned. We show that even the manipulation of highly coordinated native substrate atoms is possible and we demonstrate how this can be applied as local analytic and synthetic chemistry tools, with important consequences on surface structure research. Vertical manipulation of Xe and CO is demonstrated, leading to improved imaging with functionalized tips. With CO deliberately transferred to the tip, we have also succeeded to perform vibrational spectroscopy on single molecules. Furthermore, we describe how we have reproduced a full chemical reaction with single molecules, whereby all basic steps, namely preparation of the reactants, diffusion and association, are induced with the STM tip. Finally, we have extended the manipulation techniques to large specially designed molecules by performing lateral manipulation in constant height and realizing the principle of a conformational molecular switch.     

Single quantum dots as scanning tunneling microscope tips

We report the use of single quantum dot structures as tips on a scanning tunneling microscope (STM). A single quantum dot structure with a diameter of less than 200 nm and a height of 2 μm was fabricated by reactive ion etching. This dot was placed on a 40 μm-high mesa and mounted on the tip of a STM. The topography of large structures such as quantum wires or gold test substrates is clearly resolved with such a tip. To check the transport properties of the tip, quantum dot arrays were fabricated on resonant tunneling double barrier structures using the same process parameters. Conventional tunneling spectroscopy clearly resolved the 0D states in our samples. Using a metal substrate as second electrode such STM tips can be used to perform high resolution energy spectroscopy on single dots and free standing wire structures.     

Effects of strain field in nitrogen-mediated Co film growth on Cu(0 0 1): Segregation and electronic structure change

Growth modes of Co thin films on the both N-saturated and partially N-adsorbed Cu(0 0 1) surfaces are studied in detail. From results of the STM and XPS measurements, segregation of N atoms depending on the Co island size is concluded. This new type of atom segregation is explained by means of a lattice strain of the substrate due to the small Co island formation. A novel core-level shift of N 1s during the Co film growth is also reported. A possible influence of the lattice strain to the electronic structure of the surfactant is discussed.     

Atomistic processes and the strain distribution in the early stages of thin film growth

Structural relaxations in small Co islands on the Cu(001) surface are investigated performing atomistic calculations. We demonstrate that the strain relief at the metal interface in the early stages of heteroepitaxy is more complicated than suggested by simple considerations based on the small mismatch between the Co and Cu bulk metals. We found that the strain distribution in the surface region near the islands varies strongly on an atomic scale. The effect of strain on the shape of the Co islands is revealed. Diffusion on the top of strained islands and edge diffusion are considered. Received: 10 April 2000 / Accepted: 15 May 2000 / Published online: 7 March 2001