Methane dissociation on Ni(111): the role of lattice reconstruction

The effects of lattice motion and reconstruction on the dissociation of methane on Ni(111) are explored, using both electronic structure theory and quantum dynamical calculations. We show that during the reaction, the Ni lattice reconstructs, effectively lowering the barrier to reaction, in contrast with earlier models of this process.     

Semiclassical stochastic trajectory approach to molecule-solid surface scattering

A semiclassical stochastic trajectory (SST) approach to the sudy of collision induced transitions in gas molecule-solid surface scattering is presented. The time-dependent Schrödinger equation provides the time-evolution of the transition amplitudes for the molecular internal states. Classical mechanics is used to describe the molecule's center of mass motion as well as the surface atoms' motion — the latter through the generalized Langevin equation (GLE) method which allows the treatment of non-rigid surfaces (i.e. surface temperature effects). These quantum and classical equations of motion are coupled through the use of a time-dependent interaction potential in the Schrödinger equation and the use of the expectation value of the interaction potential in the classical equations of motion. Advantages of the SST approach include: (1) flexibility in the choice of quantum versus classical coordinates; (c) strict energy conservation for non-dissipative system; and (3) realistic treatment of surface many-body effects within the GLE. The SST technique is applied to the study of vibrational and rotational inelasticity in a model H₂Pt(111) system. As an initial test, results obtained assuming a rigid, smooth surface with an exponentially repulsive potential are compared to exact quantal and quasi-classical trajectory values to determine the accuracy and utility of the SST approach. A limited practical application is presented for the same H₂Pt(111) system but for a non-rigid surface. These results, calculated at low gas kinetic energies, indicate that surface energy transfer and surface temperature effects should be minimal for this type of system, even though the energy gaps are quite similar for rotational and phonon degrees of freedom.     

Self-organization of Cs adatoms on Ag(111) caused by quantum confinement of surface electrons on Ag clusters

The effect of quantum confinement formed by Ag nanoclusters on the self-organization of Cs adatoms on Ag(111) was studied. The existence of allowed and forbidden zones was found for the diffusion motion of Cs adatoms near and on top of the clusters. The formation of the orbits of an adatom’s motion was demonstrated for self-organization process in a Cs adatom ensemble near and on top of the clusters.     

Surface-assisted spin Hall effect in Au films with Pt impurities

We show, both experimentally and theoretically, a novel route to obtain giant room temperature spin-Hall effect due to surface-assisted skew scattering. In the experiment, we report the spin-Hall effect in Pt-doped Au films with different thicknesses t(N). The giant spin-Hall angle γ(S)=0.12±0.04 is obtained for t(N)=10 nm at room temperature, while it is much smaller for the t(N)=20 nm sample. Combined ab initio and quantum Monte Carlo calculations for the skew scattering due to a Pt impurity show γ(S)?0.1 on the Au (111) surface, while it is small in bulk Au. The quantum Monte Carlo results show that the spin-orbit interaction of the Pt impurity on the Au (111) surface is enhanced, because the Pt 5d levels are lifted to the Fermi level due to the valence fluctuation. In addition, there are two spin-orbit interaction channels on the Au (111) surface, while only one in bulk Au.     

室温下Ge(111)表面原子的协调运动

用扫描隧道显微镜观察了Ge(111)表面的由快速降温至室温而保留下来的中温相.发现除了单个Ge增原子的扩散运动外,主要的运动是发生在畴界上的Ge增原子列的开环和闭环协调运动.从实验上证实了这种最近引起很大实验和理论兴趣的运动方式.通过观察又提出了有待进一步实验和理论研究的问题.     

Direct imaging of Cu dimer formation, motion, and interaction with Cu atoms on Ag(111)

We have investigated the formation and motion of copper adatoms and addimers on Ag(111) between 6 and 25 K with low-temperature scanning tunneling microscopy. The presence of atoms and dimers alters the motion of atoms and dimers via the long-range interaction mediated by the electrons in the two-dimensional surface state band. Above 16 K, dimers show quantum rotor behavior with altered rotational behavior in the presence of an additional adatom. The most favorable diffusional motion of the dimer is identified in combination with molecular dynamics calculations to be a zigzag out-of-cell motion starting above 24 K.     

Influence of external factors on the self-organization of lead and tin telluride nanostructures on the BaF2(111) surface under conditions close to the thermodynamic equilibrium

The morphology of PbTe and SnTe nanostructures grown on BaF₂(111) substrates from the vapor phase in a vacuum under conditions close to the thermodynamic equilibrium has been investigated using atomic force microscopy. The equilibrium shape of PbTe and SnTe quantum dots and the statistical parameters of arrays of these quantum dots have been studied as a function of the thermodynamic conditions of growth, the crystal lattice mismatch between the materials of the quantum dots and substrate, and elastic properties of these materials. It has been established that, when the BaF₂(111) substrate is deformed under external mechanical loading, the self-organization of dislocations on the BaF₂(111) surface can result in the formation of a nanoscale ordered strain relief, which can be used for the fabrication of nanostructures. The morphology of this relief depends on the external load and on the temperature at which the substrate is deformed. It has been shown that the deformation effect on the surface of the substrate and light irradiation of the growth zone of nanostructures affect the nucleation of islands and kinetic processes occurring on the surface of the substrate during their growth. Using the influence of external factors on the BaF₂(111) surface under certain thermodynamic conditions, it is possible to grow SnTe and PbTe nanostructures with different morphologies: continuous epitaxial layers with a thickness of less than 10 nm, homogeneous arrays of quantum dots with a high lateral density (more than 10¹¹ cm²), quasi-periodic lateral nanostructures (nanowires), “single” and “coupled” quantum dots, and “molecules” of quantum dots.

     

Collective excitations and quantum size effects on the surfaces of Pb(111) films: An experimental study

Pb(111) film is a special system that exhibits strong quantum size effects in many electronic properties. The collective excitations, i.e., plasmons, in Pb(111) films are also expected to show signatures of the quantum size effect. Here, using high-resolution electron energy loss spectroscopy, we measured the plasmons on the surface of Pb(111) films with different film thicknesses and analyzed the plasmon dispersions. One surface plasmon branch exhibits prominent damping in the small momentum range, which can be attributed to the interaction between the top and bottom interfaces of the Pb(111)films. With the film thickness increasing, the critical momentum characterizing the damping in Pb(111) films decays not only much slower in Pb(111) films than in other metal films, and even in films with the thickness up to 40 monolayers the damping still exists. The slow decay of the surface plasmon damping, manifesting the strong quantum size effect in Pb(111) films, might be related to the strong nesting of the Fermi surface along the(111) direction.     

Monte carlo simulations of growth modes of Pb nanoislands on Si(111) surface

The growth of Pb islands on a Si(111) surface exhibits many interesting properties. For example, the self-assembled process results in a homogeneous distribution of Pb islands with uniform height. The dependence of this height on coverage and temperature can be expressed as a phase diagram [1]. In this paper we develop a model of the growth process that reflects the main features of the experimental observations and determines the key processes of quantum dot formation in a Pb/Si(111) system. The growth of islands is simulated by the Monte Carlo method. With suitably chosen parameters the model is able to reconstruct the phase diagram, via the dependence of the dynamics of Pb atoms on area and height. These dependencies are attributed to stress energy and quantum size effects.     

Density controllable growth of ZnO quantum dots by MOCVD

High quality self-assemble ZnO quantum dots (QDs) have been successfully grown on the Si(111) substrates by metalorganic chemical vapor deposition (MOCVD). The diameter of ZnO QDs is about 10 nm in average, and the densities and the sizes of ZnO QDs can be well controlled by adjusting the growth temperature, which were evident in the SEM images. The properties and stress involved in ZnO QDs are studied by X-ray diffraction. In addition, room temperature photoluminescence spectra reveal that the ZnO QDs exhibit a band gap blue shift because of the quantum confinement effects.     

Static investigation of the small clusters on the Cu(111) and Au(111) surfaces

The diffusion properties of small clusters Ag_n, Cu_n, and Au_n on the Cu(111) and Au(111) surfaces were studied using the molecular statics (MS) in order to understand the atomistic processes underlying the motion. In this work, the atomic interaction potential is modeled by a semi-empirical Embedded Atom Method (EAM), while the drag method is used to determine the static activation energy for each diffusion path. The presented results indicate that the dimer can diffuse on the (111) surface via the zig-zag and concerted motion mechanisms. The trimer diffuses according to the concerted motion mechanism. For the tetramer diffusion, the mechanism that consumes the least amount of energy is the zig-zag motion, in which only two atoms are needed for the diffusion process at one time. This allows finding a static activation energy smaller compared to the trimer diffusion.     

Temperature-dependent photoluminescence spectra of GaN epitaxial layer grown on Si(111) substrate

In this paper, the temperature-dependent photoluminescence(PL) properties of Ga N grown on Si(111) substrate are studied. The main emission peaks of Ga N films grown on Si(111) are investigated and compared with those grown on sapphire substrates. The positions of free and bound exciton luminescence peaks, i.e., FX A and D0 X peaks, of Ga N films grown on Si(111) substrates undergo red shifts compared with those grown on sapphire. This is attributed to the fact that the Ga N films grown on sapphire are under the action of compressive stress, while those grown on Si(111) substrate are subjected to tensile stress. Furthermore, the positions of these peaks may be additionally shifted due to different stress conditions in the real sample growth. The emission peaks due to stacking faults are found in Ga N films grown on Si(111) and an S-shaped temperature dependence of PL spectra can be observed, owing to the influence of the quantum well(QW) emission by the localized states near the conduction band gap edge and the temperature-dependent distribution of the photo-generated carriers.     

Evidence of Sn adatoms quantum tunneling at the alpha-Sn/Si(111) surface

We present a low-temperature scanning tunneling microscopy study of the alpha-Sn/Si(111) surface that demonstrates the fluctuating behavior of the Sn adatoms. The dynamical fluctuation model, successfully applied in describing the alpha-Sn/Ge(111) surface, is proposed for the related alpha-Sn/Si(111) surface too, although with a much lower transition temperature. In addition, a new phenomenon appears responsible for the unexpected evidence that the average oscillation frequency remains constant at temperatures lower than 15 K, in contradiction to the Arrhenius law. We explain this phenomenon as quantum tunneling of Sn adatoms.     

Simulating the motion of a quantum particle at constant temperature

The extended system method of Nosé and Hoover for the control of temperature of a classical ensemble if applied to the de Broglie-Bohm-Vigier formulation of quantum mechanics. This allows for the simulation of the motion of a quantum particle at a constant preset temperature. A specific algorithm for numerical solution of the resulting equations of motion, based on the application of the methods of molecular dynamics simulation, is provided.     

Role of the Metal/Semiconductor interface in quantum size effects: Pb /Si(111)

Self-organized islands of uniform heights can form at low temperatures on metal/semiconductor systems as a result of quantum size effects, i.e., the occupation of discrete electron energy levels in the film. We compare the growth mode on two different substrates [Si(111)- (7x7) vs Si(111)- Pb(sqrt[3]xsqrt[3] )] with spot profile analysis low-energy electron diffraction. For the same growth conditions (of coverage and temperature) 7-step islands are the most stable islands on the (7x7) phase, while 5-step (but larger islands) are the most stable islands on the (sqrt[3]xsqrt[3] ). A theoretical calculation suggests that the height selection on the two interfaces can be attributed to the amount of charge transfer at the interface.     

Electron-phonon interaction in the quantum well state of the 1 ML Na/Cu(111) system

The electron-phonon interaction in the quantum well state formed by a Na monolayer coating on Cu(111) is investigated theoretically. The calculations show that the electron-phonon coupling constant γ in this state decreases insignificantly (≈1%) compared to the value of γ for a clean copper surface. The corresponding electron-phonon contribution to the lifetime τ of the quantum well state increases by a factor of 1.5 compared to τ for the clean Cu(111) surface.     

Quasi-one-dimensional quantized states in an epitaxial Ag film on a one-dimensional surface superstructure

The in-plane energy dispersion of quantized states in an ultrathin Ag film formed on the one-dimensional (1D) surface superstructure Si(111)-(4 x 1)-In shows clear 1D anisotropy instead of the isotropic two-dimensional free-electron-like behavior expected for an isolated metal film. The present photoemission results demonstrate that an atomic layer at the film-substrate interface can regulate the dimensionality of electron motion in quantum films.     

Diffusion and pair interactions of CO molecules on Pd(111)

The diffusion and interactions of CO molecules on Pd(111) were studied by scanning tunneling microscopy. By following the random walk motion of individual molecules as a function of temperature, an activation energy barrier for diffusion of 118 +/- 5 meV was determined. The interaction between CO molecules was found to be repulsive for pairs separated by one or two Pd(111) lattice distances, and weakly attractive at a separation of sqrt[3].     

Brownian motion of a classical particle in quantum environment

The Klein–Kramers equation, governing the Brownian motion of a classical particle in a quantum environment under the action of an arbitrary external potential, is derived. Quantum temperature and friction operators are introduced and at large friction the corresponding Smoluchowski equation is obtained. Introducing the Bohm quantum potential, this Smoluchowski equation is extended to describe the Brownian motion of a quantum particle in quantum environment.     

Self-assembling of Ge quantum dots in the CaF<Subscript>2</Subscript>/Ge/CaF<Subscript>2</Subscript>/Si heteroepitaxial system and the development of tunnel-resonance diode on its basis

A CaF₂/Ge/CaF₂/Si(111) heteroepitaxial structure with Ge quantum dots was grown by molecular-beam epitaxy. A negative differential conductivity and conductivity oscillations caused by resonant hole tunneling were observed at room temperature. The energy spacing between the levels in quantum dots, as determined from the oscillation period, is 40–50 meV depending on the Ge dot size.