Regular Arrangement of Two-Dimensional Clusters of Blue Phosphorene on Ag(111)

Two-dimensional(2D) blue phosphorene with a honeycomb structure is the phosphorus analog of graphene,and is regarded as a promising 2D material with a large tunable band gap and high charge-carrier mobility.Here,using the molecular beam epitaxy method,we synthesize monolayer blue phosphorene on the Ag(111) surface.Combined with first-principles calculations,scanning tunneling microscopy measurements reveal that the blue phosphorene on the Ag(111) surface consists of 2D clusters with a buckling 1×1 lattice,arranged regularly on the Ag(111).The formation of these phosphorus clusters stems from the strain modulation induced by the lattice mismatch between blue phosphorene and the Ag(111) substrate.Moreover,x-ray photoelectron spectroscopy measurements are performed to study the instability of the blue phosphorene clusters in air.The realization of regular nanoclusters of blue phosphorene with unique sizes and morphology provides an ideal platform for the exploration of the quantum physical properties and applications of blue phosphorene.     

Adsorption behavior of Fe atoms on a naphthalocyanine monolayer on Ag(111) surface

Adsorption behavior of Fe atoms on a metal-free naphthalocyanine(H2Nc) monolayer on Ag(111) surface at room temperature has been investigated using scanning tunneling microscopy combined with density functional theory(DFT)based calculations. We found that the Fe atoms were adsorbed on the centers of H2 Nc molecules and formed Fe–H2Nc complexes at low coverage. DFT calculations show that Fe sited in the center of the molecule is the most stable configuration, in good agreement with the experimental observations. After an Fe–H2Nc complex monolayer was formed, the extra Fe atoms self-assembled to Fe clusters of uniform size and adsorbed dispersively at the interstitial positions of Fe–H2Nc complex monolayer. Therefore, the H2 Nc monolayer grown on Ag(111) could be a good template to grow dispersed magnetic metal atoms and clusters at room temperature for further investigation of their magnetism-related properties.     

Comparative study of adsorption characteristics of Cs on the GaN （0001） and GaN （0001） surfaces

The adsorption characteristics of Cs on GaN （0001） and GaN （0001） surfaces with a coverage from 1/4 to 1 monolayer have been investigated using the density functional theory with a plane-wave uttrasoft pseudopotential method based on first-principles calculations. The results show that the most stable position of the Cs adatom on the GaN （0001） surface is at the N-bridge site for 1/4 monolayer coverage. As the coverage of Cs atoms at the N-bridge site is increased, the adsorption energy reduces. As the Cs atoms achieve saturation, the adsorption is no longer stable when the coverage is 3/4 monolayer. The work function achieves its minimum value when the Cs adatom coverage is 2/4 monolayer, and then rises with Cs atomic coverage. The most stable position of Cs adatoms on the GaN （000i） surface is at H3 site for 1/4 monolayer coverage. As the Cs atomic coverage at H3 site is increased, the adsorption energy reduces, and the adsorption is still stable when the Cs adatom coverage is 1 monolayer. The work function reduces persistently, and does not rise with the increase of Cs coverage.     

Cu原子掺杂调控三聚氰胺在Au(111)表面自组装结构

The doping effect of Cu on the self-assembly film of melamine on an Au(111) surface has been investigated with scanning tunneling microscopy (STM). The evaporated Cu adatoms occupy the positions underneath the amino groups and change the hydrogen bonding pattern between the melamine molecules. Accordingly, the self-assembly structure has changed stepwise from a well-defined honeycomb into a track-like and then a triangular structure depending on the amount of Cu adatoms. The interaction between Cu adatom and melamine is moderate thus the Cu adatoms can be released upon mild heating to around 100℃. These findings are different from previous observations of either the coordination assembly or the physically trapped metal adatoms.     

Nitrogen Adatom Diffusion on a Ga－Rich GaN （0001） Surface

The diffusion of N adatoms on a Ga-rich GaN(O001) surface has been studied using density-functional theory.The configuration of Ga adatoms on a Ga-rich GaN surface has been identified. The first adlayer Ga adatoms are on top of the terminating substrate Ga atoms, and the outmost adlayer Ga adatoms exist randomly at the T4 or H3 sites. A very different diffusivity of N adatoms on a Ga-rich GaN(0001) surface has been found. The excess Ga adatoms on a GaN(0001) surface reduce the diffusion barrier by 0.75eV and influence the migration path. It seems that bilayer Ga adatoms are helpful for N atom diffusion.     

Surface diffusion of Si,Ge and C adatoms on Si （001） substrate studied the molecular dynamics simulation

Depositions of Si, Ge and C atoms onto a preliminary Si (001) substrate at different temperatures are investigated by using the molecular dynamics method. The mechanism of atomic self-assembling occurring locally on the flat terraces between steps is suggested. Diffusion and arrangement patterns of adatoms at different temperatures are observed. At 900 K, the deposited atoms are more likely to form dimers in the perpendicular [110] direction due to the more favourable movement along the perpendicular [110] direction. C adatoms are more likely to break or reconstruct the dimers on the substrate surface and have larger diffusion distances than Ge and Si adatoms. Exchange between C adatoms and substrate atoms are obvious and the epitaxial thickness is small. Total potential energies of adatoms and substrate atoms involved in the simulation cell are computed. When a newly arrived adatom reaches the stable position, the potential energy of the system will decrease and the curves turns into a ladder-like shape. It is found that C adatoms can lead to more reduction of the system energy and the potential energy of the system will increase as temperature increases.     

SURFACE PLASMON OF Ag CLUSTERS ON ALUMINA FILMS

The deposition of silver on an ordered alumina film prepared on Re(0001) surface has been studied by Auger electron spectroscopy (AES), low energy electron diffraction (LEED) and high resolution electron energy loss spectroscopy (HREELS). The results show that Ag grows initially as clusters at 90K and 300K. A red shift of the Ag surface plasmon as a function of decreasing coverage is observed, which is related to the cluster size effect. A surface plasmon characteristic of metallic Ag appears at coverages higher than 2.8 monolayer equivalent.     

STM study of selenium adsorption on Au(111) surface

Adsorption of chalcogen atoms on metal surfaces has attracted increasing interest for both the fundamental research and industrial applications. Here, we report a systematic study of selenium(Se) adsorption on Au(111) at varies substrate temperatures by scanning tunneling microscopy. At room temperature, small Se clusters are randomly dispersed on the surface. Increasing the temperature up to 200℃, a well-ordered lattice of Se molecules consisting of 8 Se atoms in ringlike structure is formed. Further increasing the temperature to 250℃ gives rise to the formation of Se monolayer with Au(111)-3~(1/2) ×3~(1/2) lattices superimposed with a quasi-hexagonal lattice. Desorption of Se atoms rather than the reaction between the Se atoms and the Au substrate occurs if further increasing the temperature. The ordered structures of selenium monolayers could serve as templates for self-assemblies and our findings in this work might provide insightful guild for the epitaxial growth of the two-dimensional transition metal dichalcogenides.     

Interface properties and electronic structures of aromatic molecules with anhydride and thio-functional groups on Ag(111) and Au(111) substrates

First-principles calculations for several aromatic molecules with anhydride and thio groups on Ag(111) and Au(111)reveal that the self-assembly structures and the interface properties are mainly determined by the functional groups of aromatic molecules. Detailed investigations of the electronic structures show that the electrons in molecular backbone are redistributed and charge transfer occurs through the bond between the metal and the functional groups after these molecules have been deposited on a metal substrate. The interaction between Ag(111)(or Au(111)) and aromatic molecules with anhydride functional groups strengthens the π bonds in the molecular backbone, while that between Ag(111)(or Au(111))and aromatic molecules with sulfur weakens the π bonds. However, the intrinsic electronic structures of the molecules are mostly conserved. The large-sized aromatic backbone has less influence on the nature of electronic structures than the small-sized one, either at the interface or at the molecules. These results are useful to build the good metal–molecule contact in molecule-based devices.     

Role of buffer layer in electronic structures of iron phthalocyanine molecules on Au(111)

We investigate the electronic structures of one and two monolayer iron phthalocyanine (FePc) molecules on Au(111) surfaces. The first monolayer FePc is lying flat on the Au(111) substrate, and the second monolayer FePc is tilted at～15° relative to the substrate plane along the nearest neighbour [101ˉ] direction with a lobe downward to the central hole of the unit cell in the first layer. The structural information obtained by first-principles calculations is in agreement with the experiment results. Furthermore, it is demonstrated that the electronic structures of FePc molecules in one-monolayer FePc/Au(111) system are perturbed significantly, while the electronic structures of FePc molecules in the second monolayer in two-monolayer FePc/Au(111) system remain almost unchanged due to the screening of the buffer layer on Au(111).     

Growth and ordering of Ni(II) diphenylporphyrin monolayers on Ag(111) and Ag/Si(111) studied by STM and LEED

The room temperature self-assembly and ordering of (5,15-diphenylporphyrinato)nickel(II) (NiDPP) on the Ag(111) and Ag/Si(111)-(√3 × √3)R30° surfaces have been investigated using scanning tunnelling microscopy and low-energy electron diffraction. The self-assembled structures and lattice parameters of the NiDPP monolayer are shown to be extremely dependent on the reactivity of the substrate, and probable molecular binding sites are proposed. The NiDPP overlayer on Ag(111) grows from the substrate step edges, which results in a single-domain structure. This close-packed structure has an oblique unit cell and consists of molecular rows. The molecules in adjacent rows are rotated by approximately 17° with respect to each other. In turn, the NiDPP molecules form three equivalent domains on the Ag/Si(111)-(√3 × √3)R30° surface, which follow the three-fold symmetry of the substrate. The molecules adopt one of three equivalent orientations on the surface, acting as nucleation sites for these domains, due to the stronger molecule-substrate interaction compared to the case of the Ag(111). The results are explained in terms of the substrate reactivity and the lattice mismatch between the substrate and the molecular overlayer.     

New phase and surface melting of Si(111) at high temperature above the (7x7)-(1x1) phase transition

The surface structure of Si(111) at high temperatures (950-1380 degrees C) has been studied with reflection high-energy electron diffraction. We have found three different surface structures: (1) A relaxed bulklike structure with adatoms of 0.25 monolayer (ML) is formed (950-1210 degrees C); (2) there is a new phase where the adatom coverage decreases to 0.20 ML (1250-1270 degrees C); (3) the surface melting occurs over 1290 degrees C. The crystalline structure below the melting layer can be explained by the vacancy model missing all adatoms and 0.45 ML of atoms in the first-double layer.     

A study of a coadsorbate surface diffusion (Pb on C/W)

The influence of a coadsorbed submonolayer (carbon) on the diffusion of adatoms (lead) along a crystal surface (tungsten) is studied in a preliminary manner by a field electron microscope technique. Experiments show that the surface diffusion of lead is strongly affected by the coadsorption of carbon: (1) The diffusion of Pb which is easy around (110) and (111) and difficult around (100) on clean tungsten becomes easier around (100) than around (110) and (111). (2) The diffusion anisotropy on the stepped surface around (100) is changed by carbon adsorption. (3) C adatoms enhance the diffusion of Pb especially around (100). (4) The mean carbon coverage required to observe these effects is only a few hundredths of a monolayer. The dependence of the surface diffusion on such small impurity coverages is discussed.     

Electronic states of a C70 monolayer on the surface of Ag(111)

We have investigated the electronic states of a C(70) monolayer on the surface of Ag(111) (1 ML C(70)/Ag(111)) using synchrotron radiation photoelectron spectroscopy and soft x-ray absorption spectroscopy techniques. The experimental data exhibit metallic properties and at least 2.6 e(-) charge transfer per C(70) molecule. The screening effect of Ag(111) on the electronic structure of C(70) is remarkable; it greatly reduces or even eliminates the on-site Hubbard energy. The work functions of the C(70) multilayer and monolayer are determined as 4.53 eV and 4.52 eV respectively. The energy levels of C(70) align with the Fermi level of the Ag(111) substrate, and the shift of the vacuum level caused by C(70) adsorption is negligible. Potassium doping indicates that 1 ML C(70)/Ag(111) can still accommodate about nine electrons and that the sample remains metallic at any doping level.     

Study of Si and C adatoms and SiC clusters on the silicon surface by the molecular dynamics method

Individual Si and C adatoms, as well as SiC clusters, on a Si surface are simulated by the molecular dynamics method in the course of investigation of the initial stages of formation of a SiC layer on silicon with the help of molecular beam epitaxy. The potential energy surfaces for Si and C adatoms on the (2 × 1) reconstructed Si(001) surface and on the nonreconstructed Si(111) surface, as well as on the Si(111) surface with a SiC cluster, are calculated and analyzed. The values of migration barriers for adatoms on these surfaces are calculated. The effect of the SiC cluster on deformation of the surface region of Si(111) and on the migration of adatoms is investigated. The deep minima observed on the potential energy surfaces immediately above a cluster and at its boundaries can trap diffusing adatoms. The distributions of stresses and strains in the silicon lattice under a cluster on the surface are studied and described.     

Surface mass transport of Ag and In on vicinal Si(111)

Mass transport of Ag and In on vicinal Si(111) has been investigated by scanning Auger microscopy (SAM). Highly anisotropic surface diffusion and surface electromigration due to direct current were observed for Ag and In adatoms on 0°−, 0.5°−, 3°− and 6°−off vicinal Si(111) surfaces. The diffusion on the intermediate layer is strongly enhanced in the direction parallel to the step edge for Ag adatoms, while it is remarkably suppressed in the direction perpendicular to the step edge for In adatoms. The activation energy of the diffusion for the Ag adatoms ranged between 0.81 and 1.3 eV, while that for In adatoms increased from 0.31 to 0.66 eV with increasing the vicinal angle. The anisotropic diffusion transport is explained in terms of the step structure and the difference in the binding energy at the step site and the terrace site.     

Novel electronically driven surface phase predicted in C/Si(111)

We predict a novel electronically driven phase for the recently created C/Si(111) surface at 1/3 monolayer coverage. Whereas the isoelectronic surface Sn/Ge(111) is a 3 x 3 distorted metal and Si/SiC(0001) is an undistorted magnetic Mott insulator, the new phase combines both features. Two of three adatoms in C/Si(111) should form a distorted (3 x 3) honeycomb sublattice, the third an undistorted insulating and magnetic triangular sublattice. The generally conflicting elements, namely, band energy, favoring distortion, and strong electron correlations favoring a Mott state, actually conspire in this case. This kind of state represents the surface analog of the Fazekas-Tosatti state in the charge density wave compound 1T-TaS2.     

Manipulation of individual water molecules on CeO2(111)

Water molecules adsorbed on the CeO(2)(111) surface are investigated by non-contact atomic force microscopy (NC-AFM) at several tip-sample temperatures ranging between 10 and 300 K. Depending on the strength of the tip-surface interaction, they appear as triangular protrusions extended over three surface oxygen atoms or as small pits at hollow sites. During NC-AFM imaging with the tip being close to the surface, occasionally the transfer of molecules between tip and surface or the tip-induced lateral displacement of water molecules to equivalent surface lattice sites is observed. We report how this situation can be exploited to produce controlled lateral manipulations. A protocol to manipulate the water molecules between pre-defined neighbouring equivalent adsorption sites of the regular lattice as well as across a surface oxygen vacancy is demonstrated.     

Gold-adatom-mediated bonding in self-assembled short-chain alkanethiolate species on the Au(111) surface

Microscopic evidence for Au-adatom-induced self-assembly of alkanethiolate species on the Au(111) surface is presented. Based on STM measurements and density-functional theory calculations, a new model for the low-coverage self-assembled monolayer of alkanethiolate on the Au(111) surface is developed, which involves the adsorbate complexes incorporating Au adatoms. It is also concluded that the Au(111) herringbone reconstruction is lifted by the alkanethiolate self-assembly because the reconstructed surface layer provides reactive Au adatoms that drive self-assembly.     

Tuning solid surfaces from hydrophobic to superhydrophilic by submonolayer surface modification

Molecular-scale understanding and manipulation of the wetting behavior of water on solids remains a fundamental challenge. Using diamond as a model system, we show that the naturally hydrophobic behavior of a hydrogen-terminated C(111) surface can be manipulated by replacing the H termination with a monolayer of adsorbate. In particular, a mixed monolayer of 1/3 Na and 2/3 F atoms leads to superhydrophilic behavior, as shown by first-principles calculations. The physical origin of the superhydrophilic behavior is attributed to the ionic nature of the Na adatoms, which mediate the right degree of binding strength between water molecules and the substrate.