Low temperature scanning force microscopy of the Si(111)-(7x7) surface

A low temperature scanning force microscope (SFM) operating in a dynamic mode in ultrahigh vacuum was used to study the Si(111)- (7x7) surface at 7.2 K. Not only the twelve adatoms but also the six rest atoms of the unit cell are clearly resolved for the first time with SFM. In addition, the first measurements of the short range chemical bonding forces above specific atomic sites are presented. The data are in good agreement with first principles computations and indicate that the nearest atoms in the tip and sample relax significantly when the tip is within a few A of the surface.     

Two-speed phase dynamics in the si(111) (7 x7)-(1 x 1) phase transition

We propose a natural two-speed model for the phase dynamics of Si(111) 7 x 7 phase transition to high-temperature unreconstructed phase. We formulate the phase dynamics by using phase-field method and adaptive mesh refinement. Our simulated results show that a 7 x 7 island decays with its shape kept unchanged, and its area decay rate is shown to be a constant increasing with its initial area. Low-energy electron microscopy experiments concerned are explained, which confirms that the dimer chains and corner holes are broken first in the transition, and then the stacking fault is remedied slowly. This phase-field method is a reliable approach to phase dynamics of surface phase transitions.     

Three-dimensional scanning force/tunneling spectroscopy at room temperature

We simultaneously measured the force and tunneling current in three-dimensional (3D) space on the Si(111)-(7 × 7) surface using scanning force/tunneling microscopy at room temperature. The observables, the frequency shift and the time-averaged tunneling current were converted to the physical quantities of interest, i.e. the interaction force and the instantaneous tunneling current. Using the same tip, the local density of states (LDOS) was mapped on the same surface area at constant height by measuring the time-averaged tunneling current as a function of the bias voltage at every lateral position. LDOS images at negative sample voltages indicate that the tip apex is covered with Si atoms, which is consistent with the Si-Si covalent bonding mechanism for AFM imaging. A measurement technique for 3D force/current mapping and LDOS imaging on the equivalent surface area using the same tip was thus demonstrated.     

Room temperature supramolecular repositioning at molecular interfaces using a scanning tunneling microscope

Individual C₆₀ molecules adsorbed on a monolayer of 4,4′-dimethyl bianthrone first grown on Cu(111) have been repositioned at room temperature with the tip of a scanning tunneling microscope. The procedure can be applied to C₆₀ without disrupting the 4,4′-dimethyl bianthrone film. Controlled supramolecular repositioning at a molecular interface has allowed us to assemble lateral C₆₀ patterns that define a bimolecular C₆₀-4,4′-dimethyl bianthrone heterojunction on Cu(111).     

Atom manipulation with the scanning tunneling microscope: nanostructuring and femtochemistry

We briefly survey our recent studies on the ‘soft’lateral manipulation of atoms and small molecules with the scanning tunneling microscope (STM), whereby mainly the tip–surface forces are employed. Repulsive (pushing) as well as discontinuous (pulling) and continuous (sliding)attractive manipulation modes could be distinguished on Cu(211) for CO molecules and metal atoms, respectively. In the case of pulling of Cu atoms on Cu(111) even finer details could be discerned: the adparticle may show various movement patterns visiting different surface sites upon applying different tip forces. Lateral manipulation also allows modifications of the Cu(211) substrate itself in an atom-by-atom manner by releasing atoms from sixfold coordinated kink sites and even sevenfold coordinated regular step sites. Furthermore, investigations concerning controled vertical manipulation with emphasis on ‘picking-up’ single CO molecules are reported. The mechanism behind vertical transfer of CO molecules relates to ultrafast chemical processes. Vertical manipulation implies, besides extending the possibilities for the build-up of nanostructures, the important possibility of creating structurally and compositionally well-defined tips, which may eventually lead to chemical sensitivity with the STM.     

Correlations between the scanning tunneling microscopy imaged configurations and the electronic structure on stepped Si(111)-( 7x7) surfaces

We have observed the dependence of the scanning tunneling microscopy (STM) imaged atom intensity within the (7x7) unit cell on stepped Si(111) as a function of the tunneling voltage. Pronounced differences from the corresponding atom intensity on the flat surface are observed for the contrast of atoms on the low versus the high side of the step and for the contrast between the faulted versus unfaulted subcells of the (7x7) structure. These differences can be accounted for by changes in the electronic structure within the (7x7) subcells adjacent to the step. Calculations of the local density of states and the STM images using a tight-binding method are in excellent agreement with the experimental results.     

Reinterpretation of the molecular O2 chemisorbate in the initial oxidation of the si(111)7 x 7 surface

The initial oxygen adsorption on the Si(111)7 x 7 surface was investigated by high-resolution x-ray absorption spectroscopy. Below 220 K, a molecular adsorption species is identified by distinctive absorption resonances due to the 1 pi(g) molecular orbitals. The molecular species is metastabilized to have a lifetime of 15-35 min at 135 K only with the presence of atomic adsorbates of more than 0. 1 ML (monolayer). It is thus clearly evidenced that the very initial adsorption is dissociative even at 100 K and the molecular species is not a precursor state. The molecular adsorption structures with the coadsorbed oxygen atoms are suggested.     

Electron-phonon interaction at the Si(111)-7 x 7 surface

It is shown that electron-phonon interaction provides a natural explanation for the unusual band dispersion of the metallic surface states at the Si(111)-(7 x 7) surface. Angle-resolved photoemission reveals a discontinuity of the adatom band at a binding energy close to the dominant surface phonon mode at h(omega0) = 70 meV. This mode has been assigned to adatom vibrations by molecular dynamics calculations. A calculation of the spectral function for electron-phonon interaction with this well-defined Einstein mode matches the data. Two independent determinations of the electron-phonon coupling parameter from the band dispersion and from the temperature-dependent phonon broadening yield similar values of lambda = 1.09 and lambda = 1.06.     

Investigating molecular charge transfer complexes with a low temperature scanning tunneling microscope

Electron donor-acceptor molecular charge transfer complexes (CTCs) formed by alpha-sexithiophene (6T) and tetrafluoro-tetracyano-quinodimethane (F4TCNQ) on a Au(111) surface are investigated by scanning tunneling microscopy, spectroscopy, and spectroscopic imaging at 6 K. New hybrid molecular orbitals are formed in the CTCs, and the highest occupied molecular orbital of the CTC is mainly located on the electron accepting F4TCNQ while the lowest unoccupied molecular orbital is predominantly positioned on the electron donating 6T. We observed the conductance switching of F4TCNQ inside CTCs, which may find potential applications in novel molecular device operations.     

Controlled lateral manipulation of single molecules with the scanning tunneling microscope

We report on the first successful lateral manipulation of molecules and controlled formation of nanostructures with the Scanning Tunneling Microscope (STM) at temperatures above 4 K as used by Eigler and collaborators. Among the first structures, we built the letters F and U forming the logo of our university at 30 K with CO molecules on a Cu(211) substrate. Our method to manipulate the molecules is analogous to that employed successfully up to now only by Eigler and co-workers. First experiences concerning the manipulation of the CO molecules on the highly anisotropic substrate are presented and the crucial role of the tip composition in imaging the CO molecules is demonstrated.     

Electronic properties of assembled islands of hydrogen-saturated silicon clusters on Si(111)-(7 x 7) surfaces studied by scanning tunneling spectroscopy

We present results of scanning tunneling spectroscopy (STS) measurements of hydrogen-saturated silicon clusters islands formed on Si(111)-( 7×7) surfaces. Nanometer-size islands of Si₆H₁₂ with a height of 0.2-4 nm were assembled with a scanning tunneling microscope (STM) using a tip-to-sample voltage larger than 3 V. STS spectra of Si₆H₁₂ cluster islands show characteristic peaks originating in resonance tunneling through discrete states of the clusters. The peak positions change little with island height, while the peak width shows a tendency of narrowing for the tall islands. The peak narrowing is interpreted as increase of lifetime of electron trapped at the cluster states. The lifetime was as short as 10^-13 s resulting from interaction with the dangling bonds of surface atoms, which prevents charge accumulation at the cluster islands. Received 30 November 2000     

Electron transmission probability across CoSi2/n-Si(111) interfaces measured with a scanning tunneling microscope

In an in situ UHV study at 77 K, a scanning tunneling microscope was used in a new constant-height mode of ballistic-electron-emission microscopy to measure the electron transmission probability across epitaxial CoSi₂ films and across CoSi₂/n-Si(111) interfaces. The conventional ballistic-electron-emission microscopy, carried out in the constant-current mode, was found to give artifacts at high tip voltages (< −2 V with sample grounded), which could be eliminated in the constant-height mode with simultaneous scanning tunneling spectroscopy.