Revisiting the structure of the p(4 x 4) surface oxide on Ag(111)

Scanning tunneling microscopy (STM) and density-functional theory are used to reexamine the structure of the renowned p(4 x 4)-O/Ag(111) surface oxide. The accepted structural model [C. I. Carlisle, Phys. Rev. Lett. 84, 3899 (2000)10.1103/PhysRevLett.84.3899] is incompatible with the enhanced resolution of the current STM measurements. An "Ag6 model" is proposed that is more stable than its predecessor and accounts for the coexistence of the p(4 x 4) and a novel c(3 x 5log3)rect phase. This coexistence is an indication of the dynamic complexity of the system that until now has not been appreciated.     

Structure of Ag(111)-p(4 x 4)-O: no silver oxide

The structure of the oxygen-induced p(4 x 4) reconstruction of Ag(111) is determined by a combination of scanning tunneling microscopy, surface x-ray diffraction, core level spectroscopy, and density functional theory. We demonstrate that all previous models of this surface structure are incorrect and propose a new model which is able to explain all our experimental findings but has no resemblance to bulk silver oxide. We also shed some light on the limitations of current density functional theories and the potential role of van der Waals interactions in the stabilization of oxygen-induced surface reconstructions of noble metals.     

Direct observation of long-range assisted formation of Ag clusters on Si(111)7 x 7

Formation of Ag clusters on reconstructed surface Si(111)7 x 7 was for the first time observed in real time during deposition by means of scanning tunneling microscopy. The sequences of images taken at room temperature show mechanisms controlling the growth and behavior of individual Ag adatoms. Obtained data reveal new details of attractive interaction between adsorbates occupying adjacent half-unit cells of the 7 x 7 reconstruction. Time evolution of growth characteristics was simulated by means of a simple model. The growth scenario observed in vivo is discussed with respect to previously reported models based on data obtained after finishing the deposition--post-mortem.     

Electrostatic potential screened by a two-dimensional electron system: a real-space observation by scanning-tunneling spectroscopy

Scanning-tunneling spectroscopy at 5 K was used to investigate the electrostatic potential profile on the Si(111)-square root of 3 x square root of 3 Ag surface at subnanometer spatial resolution. The potential was measured from an energy-level shift of electronic states on the surface. The potential images obtained reveal that the potential drops around the steps and Ag adsorbates, upon which positive charges are presumably accumulated. The profiles of the reduced potentials are explained with the screening of potential due to the charges by two-dimensional electron gas (2DEG) existing on the surface. The Friedel oscillation, which results from the screening and has a period of the half Fermi wavelength of the 2DEG, was also observed in the potential images.     

Structure determination of the Si3N4/Si(111)- (8 x 8) surface: a combined study of Kikuchi electron holography, scanning tunneling microscopy, and ab initio calculations

A comprehensive atomic model for the reconstructed surface of Si3N4 thin layer grown on Si(111) is presented. Kikuchi electron holography images clearly show the existence of adatoms on the Si3N4(0001)/Si(111)-(8x8) surface. Compared with the ab initio calculations, more than 30 symmetry-inequivalent atomic pairs in the outmost layers are successfully identified. Scanning tunneling microscopy (STM) images show diamond-shaped unit cells and nine adatoms in each cell. High-resolution STM images reveal extra features and are in good agreement with the partial charge density distribution obtained from total-energy calculations.     

Structural transformations on an oxidized Ag(111) surface

The structure of the Ag(111) surface after the adsorption of molecular oxygen at a temperature of 300 K is studied by low-temperature scanning tunneling microscopy. It is established that local surface oxide is formed at the first stage of adsorption. The subsequent adsorption of O results in the appearance of new objects with a size of 3–8 Å and a height of 1.0–1.5 Å on the Ag(111) surface, which form quasi-ordered structures with increasing degree of coating. The heating of the system obtained up to 500 K leads to a structural transition resulting in the formation of single islands of the p (4×4) phase on the surface. Surface structures are identified by a simulation based on the density functional theory.     

One-dimensional surface reconstruction as an atomic-scale template for the growth of periodically striped Ag films

The role of the In/Si(111)-(4 x 1)-In surface as an atomic-scale geometrical template for the growth of Ag thin films is clarified by scanning tunneling microscopy and low energy electron diffraction. Low-temperature grown Ag films are found to have stripe structures with a transverse periodicity equal to that of indium chains of the In/Si(111)-(4 x 1)-In. The stripes exhibit a structural transformation at the thickness of 6 monolayers (ML); this relaxation allows the stripes to persist up to a thickness as large as 30 ML (approximately = 7 nm) while maintaining their mean periodicity. We attribute this stability to a coincidental matching of the periodicity and the corrugation amplitude between the Ag film and the substrate, which is realized by periodic insertion of stacking faults into a Ag fcc crystal.     

立方相Ag_3PO_4(111)面原子几何及弛豫结构的第一性原理计算

采用平面波超软赝势方法研究了立方相Ag_3PO_4(111)面的表面能和表面原子弛豫结构.首先对Ag_3PO_4(111)面的八种不同原子终止结构的体系总能量进行计算,结果表明B种表面模型被证实为最稳定的(111)面原子几何结构.针对该表面结构,探讨了表面能和原子弛豫与模型中原子层数和真空厚度的关系,当原子层数为24层,真空厚度为0.6 nm时,表面能收敛于1.41 J/m2(LDA-CAPZ)和1.39 J/m2(GGA-PBE).表面原子弛豫后,表面两个三配位的Ag原子均向里移动,超过0.06 nm,而表面次层的O原子则均向外移动约0.0042 nm,导致弛豫后暴露在最表面的是O原子,同时表面原子的核外电子向表面内部发生转移,结构趋于稳定.这些结果为进一步深入研究Ag_3PO_4表面的光催化活性起源提供理论支持.     

立方相Ag3PO4(111)面原子几何及弛豫结构的第一性原理计算

采用平面波超软赝势方法研究了立方相Ag3PO4(111)面的表面能和表面原子弛豫结构.首先对Ag3PO4(111)面的八种不同原子终止结构的体系总能量进行计算,结果表明B种表面模型被证实为最稳定的(111)面原子几何结构.针对该表面结构,探讨了表面能和原子弛豫与模型中原子层数和真空厚度的关系,当原子层数为24层,真空厚度为0.6 nm时,表面能收敛于1.41 J/m2(LDA-CAPZ)和1.39 J/m2(GGA-PBE).表面原子弛豫后,表面两个三配位的Ag原子均向里移动,超过0.06 nm,而表面次层的O原子则均向外移动约0.0042 nm,导致弛豫后暴露在最表面的是O原子,同时表面原子的核外电子向表面内部发生转移,结构趋于稳定.这些结果为进一步深入研究Ag3PO4表面的光催化活性起源提供理论支持.     

Growth mode and interface structure of Ag on the HF-treated Si(111):H surface

A growth mode and interface structure analysis has been performed for Ag deposited at a high temperature of 300°C on the HF-treated Si(111):H surface by means of medium-energy ion scattering and elastic recoil detection analysis of hydrogen. The measurements show that Ag grows in the Volmer-Weber mode and that the Ag islands on the surface are epitaxial with respect to the substrate. The preferential azimuthal orientation is A-type only when Ag is deposited slowly. The interface does not reconstruct to the √3 × √3-Ag structure, which is normally observed for Ag deposition above 200°C on the Si(111)7 × 7 surface, but retain bulk-like structure. The presence of hydrogen at the interface is demonstrated after deposition of thick (1100 Å) Ag films. However, the amount of hydrogen at the interface is not a full monolayer. This partial desorption of hydrogen from the interface explains why the Schottky barrier heights of Ag/Si(111):H diodes are close to those of Ag/Si(111)7 × 7 and Ag/Si(111)2 × 1.     

Structural origin of the Sn 4d core level line shape in Sn/Ge(111)-(3x3)

High-resolution photoemission of the Sn 4d core level of Sn/Ge(111)-(3x3) resolves three main components in the line shape, which are assigned to each of the three Sn atoms that form the unit cell. The line shape found is in agreement with an initial state picture and supports that the two down atoms are inequivalent. In full agreement with these results, scanning tunnel microscopy images directly show that the two down atoms are at slightly different heights in most of the surface, giving rise to an inequivalent-down-atoms (3x3) structure. These results solve a long-standing controversy on the interpretation of the Sn 4d core-level line shape and the structure of Sn/Ge(111)-(3x3).     

SnPc在Ag(111)表面吸附特性的第一性原理研究

采用第一性原理研究了SnPc分子在Ag(111)表面的吸附构型和电子结构. Sn-up和Sn-down两种优化的吸附构型与实验测量结果非常吻合,SnPc以Sn-down构型吸附在Ag(111)表面显得更稳定. Sn原子在两种吸附构型之间转换所需要能量与转换方向有关,由Sn-up向Sn-down构型转换时需翻越一个1.68 eV的能垒,反之需要2.17 eV. 扫描隧道显微镜理论模拟图像给出实验观测结果的主要特征,Sn-up分子的中心处为一个亮斑,而Sn-down分子中心为一个空洞. 计算结果验证了实验提出的Sn原子吸附位置的转换机理.     

Fermi gap stabilization of an incommensurate two-dimensional superstructure

The compressed, incommensurate approximately (9.5 x 9.5) moire superstructure of the Ag monolayer on Cu(111) displays a filled surface state band with a Fermi energy gap at the Brillouin zone boundary. By contrast, the surface band is gapless for the less compressed, commensurate (9 x 9) moire of two Ag layers. A simple estimate of the energy gain rendered by opening this gap gives a value similar to the elastic energy change required to modify the commensurate structure, thereby suggesting that the approximately (9.5 x 9.5) incommensurate phase is stabilized by such a gap opening. The possible presence of a charge density wave state is discussed.     

Effect of driving frequency on the structure of silicon grown on Ag(111) films by very-high-frequency magnetron sputtering

The effect of driving frequency on the structure of silicon grown on Ag(111) film is investigated, which was prepared by using the very-high-frequency(VHF)(40.68 MHz and 60 MHz) magnetron sputtering. The energy and flux density of the ions impinging on the substrate are also analyzed. It is found that for the 60-MHz VHF magnetron sputtering, the surface of silicon on Ag(111) film exhibits a small cone structure, similar to that of Ag(111) film substrate, indicating a better microstructure continuity. However, for the 40.68-MHz VHF magnetron sputtering, the surface of silicon on Ag(111) film shows a hybrid structure of hollowed-cones and hollowed-particles, which is completely different from that of Ag(111)film. The change of silicon structure is closely related to the differences in the ion energy and flux density controlled by the driving frequency of sputtering.     

Using polarity for engineering oxide nanostructures: structural phase diagram in free and supported MgO(111) ultrathin films

Using an ab initio total energy approach, we study the stability of free and Ag(111)-supported MgO(111) ultrathin films. We unravel a novel microscopic mechanism of stabilization of polar oxide orientations, based on a strong modification of the MgO structural phase diagram with respect to the bulk material. We predict that, at low thickness, films which are either unsupported or deposited on Ag(111) display a graphitelike Bk structure rather than the expected rocksalt one. Our results provide a consistent interpretation of recent experimental findings, exemplify the efficiency of this novel stabilization mechanism, and suggest new methods to engineer oxide nanostructures.     

Formation of Two-Dimensional AgTe Monolayer Atomic Crystal on Ag(111) Substrate

We report on the formation of two-dimensional monolayer AgTe crystal on Ag(111) substrates. The samples are prepared in ultrahigh vacuum by deposition of Te on Ag(111) followed by annealing. Using a scanning tunneling microscope(STM) and low electron energy diffraction(LEED), we investigate the atomic structure of the samples.The STM images and the LEED pattern show that monolayer AgTe crystal is formed on Ag(111). Four kinds of atomic structures of AgTe and Ag(111) are observed:(i) flat honeycomb structure,(ii) bulked honeycomb,(iii)stripe structure,(iv) hexagonal structure. The structural analysis indicates that the formation of the different atomic structures is due to the lattice mismatch and relief of the intrinsic strain in the AgTe layer. Our results provide a simple and convenient method to produce monolayer AgTe atomic crystal on Ag(111) and a template for study of novel physical properties and for future quantum devices.     

Ag growth on Si(111) with an Sb surfactant investigated by scanning tunneling microscopy

We have investigated a room-temperature growth mode of ultrathin Ag films on a Si(111) surface with an Sb surfactant using STM in a UHV system. On the Sb-passivated Si surface, small sized islands were formed up to 1.1 ML. Flat Ag islands were dominant at 2.1 ML, coalescing into larger islands at 3.2 ML. Although the initial growth mode of Ag films on the Sb-terminated Si(111) surface was Volmer-Weber (island growth), the films were much more uniform than Ag growth on clean (Si(111) at the higher coverages. From the analysis of STM images of Ag films grown with and without an Sb surfactant, the uniform growth of Ag films using an Sb surfactant appears to be caused by the kinetic effects of Ag on the preadsorbed Sb layer. Our STM results indicated that Sb suppresses the surface diffusion of Ag atoms and increases the Ag-island density. The increased island density is believed to cause coalescence of Ag islands at higher coverages of Ag, resulting in the growth of atomically flat and uniform Ag islands on the Sb surfactant layer.     

Ag(100)表面氧吸附的密度泛函理论和STM图像研究

用密度泛函理论研究了氧原子的吸附对于Ag(100)表面结构和电子态的影响.通过PAW总能计算研究了p(1×1)、c(2×2)和(2^1/2×22^1/2)R45°等几种原子氧覆盖度下的吸附结构，以及在上述结构下Ag(100)表面的弛豫特性、吸附能量、功函数等一系列物理量.研究表明：在(2^1/2×22^1/2)R45°-2O吸附Ag(100)表面的情况下，每格两列就会缺失     

Ag(100)表面氧吸附的密度泛函理论和STM图像研究

用密度泛函理论研究了氧原子的吸附对于Ag(100)表面结构和电子态的影响.通过PAW总能计算研究了p(1×1)、c(2×2)和(2^1/2×22^1/2)R45°等几种原子氧覆盖度下的吸附结构,以及在上述结构下Ag(100)表面的弛豫特性、吸附能量、功函数等一系列物理量.研究表明：在(2^1/2×22^1/2)R45°-2O吸附Ag(100)表面的情况下,每格两列就会缺失 关键词： Ag(100)表面氧吸附 缺列再构 STM图像     

Single atomic manipulation and writing with scanning tunnelling microscopy at low temperatures

In the work reported in this paper,we have used a low-temperature scanning tunnelling microscope (LT-STM) system to manipulate accurately single atoms.We show how we can use a LT-STM to image and modify a bulk Ag(111) surface and manipulate Ag atoms from substrate and evaporated adsorbates on Ag(111) substrates.We present a synergistic combination of SM-induced modification and ordered arrays of nanometre-scale structures.In particular,we demonstrate the ability to modify Ag atomic nanometre structures on the Ag(111) substrate,and some English letters and a Chinese character can be written by single Ag atoms coming from the substrate and evaporated adsorbates on Ag(111),In this way ,we supply an effective basis to explore the fundamental physical properties of a nanometre structure and to develop nanotechnology with a bottom-up approach,