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.     

Giant alkali-metal-induced lattice relaxation as the driving force of the insulating phase of alkali-metal/Si(111):B

Ab initio density-functional theory calculations, photoemission spectroscopy (PES), scanning tunneling microscopy, and spectroscopy (STM, STS) have been used to solve the 2sqrt[3]×2sqrt[3]R30 surface reconstruction observed previously by LEED on 0.5 ML K/Si:B. A large K-induced vertical lattice relaxation occurring only for 3/4 of Si adatoms is shown to quantitatively explain both the chemical shift of 1.14 eV and the ratio 1/3 measured on the two distinct B 1s core levels. A gap is observed between valence and conduction surface bands by ARPES and STS which is shown to have mainly a Si-B character. Finally, the calculated STM images agree with our experimental results. This work solves the controversy about the origin of the insulating ground state of alkali-metal/Si(111):B semiconducting interfaces which were believed previously to be related to many-body effects.     

Direct observation of sn adatoms dynamical fluctuations at the Sn/Ge(111) surface

The well-known low-temperature phase transition sqrt[3]xsqrt[3] to 3x3 for the 1/3 monolayer of Sn adatoms on the Ge(111) surface has been studied by scanning tunneling microscopy. The STM tip was used as a probe to record the tunneling current as a function of time on top of the Sn adatoms. The presence of steps on the current-time curves allowed the detection of fluctuating Sn atoms along the direction vertical to the substrate. We discuss the effect of temperature and surface defects on the frequency of the motion, finding consistency with the dynamical fluctuations model.     

Low temperature disordered phase of alpha-Pb/Ge(111)

A new structural phase transition has been observed at low temperature for the one-third of a monolayer (alpha phase) of Pb on Ge(111) using a variable-temperature scanning tunneling microscope. The well-known (sqrt[3] x sqrt[3])R30 degrees to (3 x 3) transition is accompanied by a new structural phase transition from (3 x 3) to a disordered phase at approximately 76 K. The formation of this "glasslike" phase is a consequence of competing interactions on different length scales.     

Direct observation of a (3 x 3) phase in alpha-Pb/Ge(111) at 10 K

We have investigated the recently reported structural phase transition at low temperature (LT) for alpha-Pb/Ge(111) [from a (3 x 3) symmetry to a disordered phase] using scanning tunneling microscopy (STM). By tracking exactly the same surface regions with atomic resolution while varying the sample temperature from 40 to 140 K, we have observed that substitutional point defects are not mobile, in clear contrast to previous assumptions. Moreover, STM data measured at the lowest temperatures ever reported for this system (10 K) show that while filled-state images display the apparent signature of a glassy phase with no long-range order, in empty-state images honeycomb patterns with (3 x 3) periodicity, and not distinguishable from data measured at much higher temperatures, are clearly resolved. These new observations cast serious doubts on the nature and/or on the existence of a disordered phase at LT.     

Bias voltage dependent shift of the atomic-scale structure of a Ge(111)-(2 × 1) reconstructed surface measured by low temperature scanning tunneling microscopy

The results of low temperature scanning tunneling microscopy (STM) investigations of a clean Ge(111) surface are presented. Bias dependent shifts of the atomic-scale structure caused by the (2 × 1) reconstruction of the Ge(111) surface are observed. A detailed comparison of experimental data with theoretical predictions based on the π-bonded chain model indicates that inelastic tip-sample interaction plays a significant role in STM imaging of the Ge(111)-(2 × 1) reconstructed surface. The text was submitted by the authors in English.     

La0.67Ca0.33MnO3(001)薄膜表面结构的扫描隧道显微术研究

利用Scanning Tunneling Microscope(STM)和Scanning Tunneling Spectroscopy(STS)技术研究了La_0.67Ca_0.33MnO₃(001)表面性质,研究发现表面呈现多相分离现象,在锰氧终端面观察到了绝缘性的( 2 × 2 )R45°重构表面和金属性的(1×1)重构表面,在镧钙氧终端面,观察到了表面呈现条纹状结构.La_0.67Ca_{0.33 关键词： 镧钙锰氧薄膜 终端面 绝缘金属转变}     

Disproportionation phenomena on free and strained Sn/Ge(111) and Sn/Si(111) surfaces

Distortions of the sqrt[3]x sqrt[3] Sn/Ge(111) and Sn/Si(111) surfaces are shown to reflect a disproportionation of an integer pseudocharge, Q, related to the surface band occupancy. A novel understanding of the (3 x 3)-1U ("1 up, 2 down") and 2U ("2 up, 1 down") distortions of Sn/Ge(111) is obtained by a theoretical study of the phase diagram under strain. Positive strain keeps the unstrained value Q=3 but removes distortions. Negative strain attracts pseudocharge from the valence band causing first a (3 x 3)-2U distortion (Q=4) on both Sn/Ge and Sn/Si, and eventually a (sqrt[3] x sqrt[3])-3U ("all up") state with Q=6. The possibility of a fluctuating phase in unstrained Sn/Si(111) is discussed.     

Surface soft phonon and the sqrt[3] x sqrt[3] <--> 3x3 phase transition in Sn/Ge(111) and Sn/Si(111)

Density functional theory calculations show that the reversible Sn/Ge(111) sqrt[3]xsqrt[3]<-->3x3 phase transition can be described in terms of a surface soft phonon. The isovalent Sn/Si(111) case does not display this transition since the sqrt[3]xsqrt[3] phase is the stable structure at low temperature, although it presents a partial softening of the 3x3 surface phonon. The rather flat energy surfaces for the atomic motion associated with this phonon mode in both cases explain the experimental similarities found at room temperature between these systems. The driving force underlying the sqrt[3]xsqrt[3]<-->3x3 phase transition is shown to be associated with the electronic energy gain due to the Sn dangling bond rehybridization.     

Surface phase transitions induced by electron mediated adatom-adatom interaction

We propose that the indirect adatom-adatom interaction mediated by the conduction electrons of a metallic surface is responsible for the sqrt[3]xsqrt[3]<==>3x3 structural phase transitions observed in Sn/Ge (111) and Pb/Ge (111). When the indirect interaction overwhelms the local stress field imposed by the substrate registry, the system suffers a phonon instability, resulting in a structural phase transition in the adlayer. Our theory is capable of explaining all the salient features of the sqrt[3]xsqrt[3]<==>3x3 transitions observed in Sn/Ge (111) and Pb/Ge (111), and is in principle applicable to a wide class of systems whose surfaces are metallic before the transition.     

Effect of H2O chemisorption on passivation of Ge(100) surface studied by scanning tunneling microscopy

The electronic passivation of a Ge(100) surface, via the chemisorption of H₂O at room temperature (RT), and the temperature dependence of H₂O coverage were investigated using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). With a saturation H₂O dose at RT, a highly-ordered structure, due to the dissociative chemisorption of H₂O, was observed on a Ge(100) surface with a coverage of 0.85 monolayers (ML). Annealing the room temperature H₂O-dosed Ge surface to 175 °C decreased the coverage of H₂O to 0.6 ML. Further annealing at 250 °C decreased the coverage of H₂O sites to 0.15 ML, and the surface reconstruction of Ge dimers was observed over much of the surface. Annealing above 300 °C induced Ge suboxide structures, similar to the oxygen-dosed Ge surface. STS measurements confirmed that the surface dangling bond states near Fermi energy are removed by the H₂O chemisorption because the dangling bonds of Ge atoms are terminated by ―OH and ―H. The H₂O pre-dose at room temperature provides a template for the ultrathin passivation of Ge(100) surface via atomic layer deposition (ALD) at RT, since near monolayer nucleation can be obtained with a 1/2 hydroxylated and 1/2 hydrogenated Ge surface.     

Semiconducting surface reconstructions of p-type Si(100) substrates at 5 K

We report scanning tunneling microscopy (STM) studies of the technologically important Si(100) surface that reveal at 5 K the coexistence of stable surface domains consisting of the p(2 x 1) reconstruction along with the c(4 x 2) and p(2 x 2) reconstructions. Using highly resolved tunneling spectroscopic measurements and tight binding calculations, we prove that the p(2 x 1) reconstruction is asymmetric and determine the mechanism that enables the contrast variation observed in the formation of the bias-dependent STM images for this reconstruction.     

Formation and local electronic structure of Ge clusters on Si（111）-7×7 surfaces

We report the formation and local electronic structure of Ge clusters on the Si(111)-7$\times $7 surface studied by using variable temperature scanning tunnelling microscopy (VT-STM) and low-temperature scanning tunnelling spectroscopy (STS). Atom-resolved STM images reveal that the Ge atoms are prone to forming clusters with 1.0~nm in diameter for coverage up to 0.12~ML. Such Ge clusters preferentially nucleate at the centre of the faulted-half unit cells, leading to the `dark sites' of Si centre adatoms from the surrounding three unfaulted-half unit cells in filled-state images. Bias-dependent STM images show the charge transfer from the neighbouring Si adatoms to Ge clusters. Low-temperature STS of the Ge clusters reveals that there is a band gap on the Ge cluster and the large voltage threshold is about 0.9~V.     

Alignment of Ge nanoislands on Si(111) by Ga-induced substrate self-patterning

A novel mechanism is described which enables the selective formation of three-dimensional Ge islands. Submonolayer adsorption of Ga on Si(111) at high temperature leads to a self-organized two-dimensional pattern formation by separation of the 7 x 7 substrate and Ga/Si(111)-(square root[3] x square root[3])-R30 degrees domains. The latter evolve at step edges and domain boundaries of the initial substrate reconstruction. Subsequent Ge deposition results in the growth of 3D islands which are aligned at the boundaries between bare and Ga-covered domains. This result is explained in terms of preferential nucleation conditions due to a modulation of the surface chemical potential.     

Growth mechanism and morphology of Ge on Pb covered Si(111) surfaces

We study the mechanism and surface morphology in epitaxial growth of Ge on Pb covered Si(111) using a scanning tunneling microscope (STM). We find that Ge adatoms have a very large diffusion length at room temperature. The growth is close to perfect layer-by-layer for the first two bilayers. Surface roughness increases gradually with the film thickness, but no 3D islands are found at room temperature. For growth at 200°C, 3D Ge islands appear after completion of the second bilayer. At room temperature, we believe, the Pb layer enhances surface diffusion and the descending-step motion of Ge adatoms, but the ascending-step motion is hindered and thus 3D island growth is suppressed.     

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.     

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.     

Determination of the Sn 4d line shape of the Sn/Ge(111) radical3 x radical3 and 3x3 surfaces

The Sn 4d line shapes of the Sn/Ge(111) sqrt[3]xsqrt[3] and 3x3 surfaces are currently under debate. By employing LEED, core-level, and valence band spectroscopy we have been able to determine the correct Sn 4d line shapes for these surfaces. Contrary to a recent study we conclude that the majority of the earlier reports present line shapes close to the correct ones. At 70 K we identify three 4d components in the 3x3 spectrum, two of which are identified with the two types of Sn atoms in the 3x3 cell. The third component is attributed to Sn atoms surrounding Ge substitutional defects.     

Phonon softening,chaotic motion,and order-disorder transition in Sn/Ge(111)

The phonon dynamics of the Sn/Ge(111) interface is studied using high-resolution helium atom scattering and first-principles calculations. At room temperature we observe a phonon softening at the Kmacr; point in the (sqrt[3]xsqrt[3])R30 degrees phase, associated with the stabilization of a (3x3) phase at low temperature. That phonon band is split into three branches in the (3x3) phase. We analyze the character of these phonons and find out that the low- and room-temperature modes are connected via a chaotic motion of the Sn atoms. The system is shown to present an order-disorder transition.     

One-dimensional diffusion of vacancies on Sr/Si(100)-c(2×4) surface

An Sr/Si(100)-c(2×4) surface is investigated by high-resolution scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). The semiconductor property of this surface is confirmed by STS. The STM images of this surface shows that it is bias-voltage dependent and an atomic resolution image can be obtained at an empty state under a bias voltage of 1.5 V. Furthermore, one-dimensional (1D) diffusion of vacancies can be found in the room-temperature STM images. Sr vacancies diffuse along the valley channels, which are constructed by silicon dimers in the surface. Weak interaction between Sr and silicon dimers, low metal coverage, surface vacancy, and energy of thermal fluctuation at room temperature all contribute to this 1D diffusion.