On the microscopic origin of the kinetic step bunching instability on vicinal Si(0 0 1)

A scanning tunneling microscopy/atomic force microscopy study is presented of a kinetically driven growth instability, which leads to the formation of ripples during Si homoepitaxy on slightly vicinal Si(0 0 1) surfaces miscut in [1 1 0] direction. The instability is identified as step bunching, that occurs under step-flow growth conditions and vanishes both during low-temperature island growth and at high temperatures. We demonstrate, that the growth instability with the same characteristics is observed in two dimensional kinetic Monte Carlo simulation with included Si(0 0 1)-like diffusion anisotropy. The instability is mainly caused by the interplay between diffusion anisotropy and the attachment/detachment kinetics at the different step types on Si(0 0 1) surface. This new instability mechanism does not require any additional step edge barriers to diffusion of adatoms. In addition, the evolution of ripple height and periodicity was analyzed experimentally as a function of layer thickness. A lateral “ripple-zipper” mechanism is proposed for the coarsening of the ripples.     

Eu- and Yb-induced reconstructions on a vicinal Si(1 0 0) surface

Early stages of rare-earth metal (Yb and Eu) growth on a vicinal, single-domain Si(1 0 0)2 × 1 surface have been studied in the coverage range of 0.1-0.3 monolayer (ML) by low energy electron diffraction, scanning tunneling microscopy, and synchrotron radiation photoemission spectroscopy. We show that Yb induces the 2 × 3 periodicity in the whole range of coverage studied. The 2 × 3 reconstruction coexists with the local 3 × 2/4 × 2 structure at about 0.2 ML of Yb. In contrast, Eu forms the 3 × 2 periodicity at 0.1-0.2 ML, whereas this structure is converted into the 2 × 3 phase at about 0.3 ML. The atomic arrangement and electronic properties of these reconstructions and the adsorbate-mediated modification of surface morphology are investigated.     

Evidence for diffusion-limited kinetics during electromigration-induced step bunching on Si(1 1 1)

We have measured how the initial terrace width l₀ on vicinal Si(1 1 1) surfaces influences the rate of step bunching and the minimum terrace width within a bunch when direct-current heated at 940-1290 °C. A comparison of this data with analytic solutions and numerical simulations of the conventional “sharp-step” model give strong evidence that the kinetic length d is relatively small (d < ∼20 nm) in both temperature regime I (∼850-950 °C) and regime III (∼1200-1300 °C), in which step-down current is required for step bunching. This indicates that surface mass transport is diffusion-limited in both regimes I and III when l₀ > 20 nm, and hence that the adatom attachment- and terrace diffusion-hopping rates are of comparable magnitude. We also observe similar scaling with initial terrace width in temperature regime II (∼1040-1190 °C), in which step-up current is required for bunching, suggesting a similar step bunching mechanism in all three temperature regimes.     

Orientation and structure of triple step staircase on vicinal Si(1 1 1) surfaces

The vicinal Si(1 1 1) surface, inclined towards the direction, was investigated by scanning tunnelling microscopy and spot profile analysing low energy electron diffraction. It has been established that the surface, consisting of regularly spaced triple steps and (1 1 1) terraces with a width equal to that of a single unit cell of the Si(1 1 1)-7 × 7 surface structure, has the (7 7 10) orientation. An atomic model of the triple step is proposed.     

Stable surface termination on vicinal 6H-SiC(0 0 0 1) surfaces

Ordered nanofacet structures on vicinal 6H-SiC(0 0 0 1) surfaces, consisting of pairs of a (0 0 0 1) basal plane and a facet, are investigated in terms of stable surface stacking of the (0 0 0 1) basal planes. The surface termination of S3 (or S3*), i.e., ABC (or A*C*B*), was suggested by a structural model based on quantized step-bunching, which typically gives a one-unit-cell bunched step configuration at the facet. Here, we evaluate the surface termination at basal planes covered with a layer of silicon oxynitride by means of quantitative low-energy electron diffraction (LEED) analysis combined with scanning tunneling microscopy (STM), and show the validity of the structural model proposed.     

Morphological evidence for surface pre-melting on Si(1 1 1)

We present what we believe to be the first morphological evidence for the occurrence of surface pre-melting on the Si(1 1 1) surface. Our results complement the extensive previous evidence from diffraction and ion scattering techniques for the presence of pre-melted (liquid-like) layers on Si(1 1 1) below the bulk melting temperature and also suggest how atomic steps are involved in the initiation of such layers. Our results are based on atomic force microscopy studies of morphologies that are preserved when surfaces are annealed in a range of high temperatures and then rapidly cooled to room temperature for observation. A unique feature of the experiments is the use of specially prepared atomically flat or very low step density surfaces; this allows us to see how the liquid-like morphologies are associated with the steps and also allows the high temperature structures to survive the cooling process without being absorbed into the steps which normally would exist on a surface vicinal to (1 1 1). Quenched-in structures ascribed to pre-melting also act as sinks for diffusing ‘excess’ adatoms generated by the (1 × 1) to (7 × 7) transition and this leads to the formation of dendritic islands.     

Reconstruction on Au(0 0 1) vicinal surfaces in UHV and in sulfuric acid solution

Using scanning tunneling microscopy we have studied the reconstruction on Au(1 1 n) surfaces in ultra-high vacuum and in electrolyte. Similar to the well-known (5 × 20) quasi-“hex” reconstruction on Au(0 0 1), the reconstruction consists of parallel reconstruction lines along the steps indicative of a higher atom density in the first Au layer. In contrast to nominally flat Au(0 0 1) where the reconstruction period is 1.44 nm, we find considerably larger reconstruction periods (1.8−1.96 nm) on incidentally flatter regions of nominal Au(1 1 9), Au(1 1 11), and Au(1 1 17) surfaces. The enlarged reconstruction period is attributed to the stress field on stepped surfaces. In agreement with previous studies we find a reconstruction free zone at the step edges.     

Scaling behavior of island density in submonolayer growth of CaF2 on vicinal Si(1 1 1)

We have studied the scaling behavior of two-dimensional island density during submonolayer growth of CaF₂ on vicinal Si(1 1 1) surfaces using scanning tunneling microscopy. We have analyzed the morphology of the Si(1 1 1) surfaces where CaF₂ partial monolayers with coverages of about 0.1 monolayer are deposited at ∼600 °C. The number density of terrace nucleated islands increases with substrate terrace width l as ∼l⁴ in a low island density regime. This scaling behavior is consistent with predictions for the case of the irreversible growth of islands.     

Vacancy charging on Si(1 1 1)-(7 × 7) investigated by density functional theory

The structure and energetics of charged vacancies on Si(1 1 1)-(7 × 7) are investigated using density functional theory calculations supplemented by estimates of ionization entropy. The calculations predict multiple possible charge states for the unfaulted edge vacancy in the adatom layer, although the −2 state is most stable on real Si(1 1 1) surfaces for which the Fermi level lies near the middle of the band gap.     

Theoretical study on the temperature-induced structural transition of the Si(1 1 3) surface

The temperature-induced structural transition of the Si(1 1 3) surface is investigated by ab initio calculations. In this study, it is found that the room-temperature phase and the high-temperature phase have the 3 × 2 interstitial structure and the 3 × 1 interstitial structure, respectively. The existence of the 3 × 2 and 3 × 1 interstitial structures is supported by the analysis of scanning tunneling microscopy (STM) images and the calculation of surface core level shifts using final state pseudopotential theory. The theoretical STM images of interstitial structures are in good agreement with the STM images suggested by experiments. The analysis of STM images provides an insight into the characteristics of domain boundaries observed frequently in experiments. It is also found that the domain boundary can be formed by local 3 × 1 interstitial structures on the 3 × 2 interstitial surface. The theoretical analysis of the surface core level shifts reveals that the surface core levels in experiment originate from the interstitial structures. The lowest values in the surface core level shifts are found to be associated with the 2p core level shifts of the interstitial atoms.     

Impact of the growth on the stability–instability transition at Si (111) during step bunching induced by electromigration

The central result of this work is the definite proof that the mechanisms of the direct current induced step bunching in the middle and high temperature domains are different. We used the recently developed technique for reflection electron microscopy (REM) observation of Si surfaces during equilibrium and during crystal growth to document the impact of the growth on the process of step bunching induced by direct current heating of an Si crystal. We found completely different effects of crystal growth on the stability of the vicinal surfaces in the two temperature domains 1160–1240°C and 1260–1320°C. In the high temperature domain step bunching takes place at step-down direction of the electric current during sublimation, equilibrium and growth; whereas in the 1160–1240°C domain bunching takes place at step-up current during sublimation and at step-down current during growth. These findings support the concept of local mass transport in the high temperature domain — the surface migration of adatoms is effectively interrupted at each step by a high rate exchange between the adlayer and the crystal phase. At 1160–1240°C the mass transport is global — adatoms easily cross the steps without taking part in the crystal–adlayer exchange. Since earlier studies of other researchers support the concept of local mass transport in the low temperature domain, 900–1050°C, a difficult question arises — why do the properties of the steps, with respect to the mass transport over the crystal surface, have a temperature dependence which is not monotonous? To explain the transition from local mass transport in the low temperature domain to global mass transport in the middle temperature domain we advance a hypothesis for a transition from a low temperature state of adsorption (Takayanagi-like adatoms, existing above the (7×7)↔(1×1) transition) to a high temperature state of adsorption (adatom with three dangling bonds) with much lower activation energy for desorption.     

Au island growth on a Si(1 1 1) vicinal surface

Au island nucleation and growth on a Si(1 1 1) 7 × 7 vicinal surface was studied by means of scanning tunneling microscopy. The surface was prepared to have a regular array of step bunches. Growth temperature and Au coverage were varied in the 255-430 °C substrate temperature range and from 1 to 7 monolayers, respectively. Two kinds of islands are observed on the surface: Au-Si reconstructed islands on the terraces and three-dimensional (3D) islands along the step bunches. Focusing on the latter, the dependence of island density, size and position on substrate temperature and on Au coverage is investigated. At 340 °C and above, hemispherical 3D islands nucleate systematically on the step edges.     

Diffusion of Pb adatom and ad-dimer on Si(1 0 0) from ab initio studies

The diffusion pathways of Pb adatoms and ad-dimers on Si(1 0 0) are investigated by first-principles calculations. Pb adatoms are found to diffuse on top of the Si(1 0 0) dimer row with an energy barrier of 0.31 eV. However, Pb dimers are energetically more stable. Pb dimers on top of the dimer row have a high energy barrier (0.95 eV) to rotate from the lowest energy configuration to the orientation parallel to the underlying Si(1 0 0) dimer row. Once the ad-dimer is oriented parallel to Si(1 0 0) dimer row, they can diffuse along the dimer row with an energy barrier of only 0.32 eV.     

Growth and surface alloying of Fe on Pt(9 9 7)

The growth of ultra-thin layers of Fe on the vicinal Pt(9 9 7) surface is studied by thermal energy He atom scattering (TEAS) and Auger Electron Spectroscopy (AES) in the temperature range between 175 K and 800 K. We find three distinct regimes of qualitatively different growth type. Below 450 K the formation of a smooth first monolayer, at and above 600 K the onset of bulk alloy formation, and at intermediate temperature 500-550 K the formation of a surface alloy. Monatomic Fe rows are observed to decorate the substrate steps between 175 K and 500 K. The importance of the high step density is discussed with respect to the promotion of smooth layer growth and with respect to the alloying process and its kinetics.     

A two-region diffusion model for current-induced instabilities of step patterns on vicinal Si(1 1 1) surfaces

We study current-induced step bunching and wandering instabilities with subsequent pattern formations on vicinal surfaces. A novel two-region diffusion model is developed, where we assume that there are different diffusion rates on terraces and in a small region around a step, generally arising from local differences in surface reconstruction. We determine the steady state solutions for a uniform train of straight steps, from which step bunching and in-phase wandering instabilities are deduced. The physically suggestive parameters of the two-region model are then mapped to the effective parameters in the usual sharp step models. Interestingly, a negative kinetic coefficient results when the diffusion in the step region is faster than on terraces. A consistent physical picture of current-induced instabilities on Si(1 1 1) is suggested based on the results of linear stability analysis. In this picture the step wandering instability is driven by step edge diffusion and is not of the Mullins–Sekerka type. Step bunching and wandering patterns at longer times are determined numerically by solving a set of coupled equations relating the velocity of a step to local properties of the step and its neighbors. We use a geometric representation of the step to derive a nonlinear evolution equation describing step wandering, which can explain experimental results where the peaks of the wandering steps align with the direction of the driving field.     

Irreversible structural transformation of Si(1 1 4)-2 × 1 induced by subsurface carbon

Using scanning tunneling microscopy (STM), it has been found that the reconstruction of Si(1 1 4) is transformed irreversibly from a 2 × 1 structure composed of dimer (D), rebonded atom (R), and tetramer (T) rows (phase A) to a different kind of 2 × 1 structure composed of D, T, and T rows (phase B) by C incorporation. It has been confirmed by high-resolution synchrotron core-level photoemission spectroscopy (PES) that such an irreversible structural transformation is due to stable subsurface C atoms. They induce anisotropic compressive stress on the surface, which results in insertion of Si dimers to an R row to form a T row.     

Reflection high-energy positron diffraction pattern from a Si(1 1 1)-(7 × 7) surface

We have investigated the feature of reflection high-energy positron diffraction (RHEPD) pattern from a Si(1 1 1)-(7 × 7) surface. The RHEPD pattern observed in the total reflection condition is quite different from the conventional reflection high-energy electron diffraction (RHEED) pattern. This fact is attributed to the different penetration depths of positrons and electrons. We show that the intensity distribution of RHEPD pattern is reproduced considering the dimer-adatom-stacking fault (DAS) model with optimized atomic positions and scattering potentials of adatoms and rest atoms.     

Atomic structure of the Si(5 5 12)-2 × 1 surface

Based on the results of scanning tunneling microscopy studies of the reconstructed Si(5 5 12)-2 × 1 surface, its atomic structure has been found. It turns out that Si(5 5 12)-2 × 1 consists of four one-dimensional structures: honeycomb (H) chain, π-bonded H′ (π) chain, dimer-adatom (D/A) row, and tetramer (T) row. Its period is composed of three subunits, i.e., (i) (3 3 7) unit with a D/A row [D(3 3 7)], (ii) (3 3 7) unit with a T row [T(3 3 7)], and (iii) (2 2 5) unit with both a D/A and a T row. Two kinds of adjacent subunits, T(3 3 7)/D(3 3 7) and D(3 3 7)/(2 2 5), are divided by H chains with 2× periodicity due to buckling, while one kind of adjacent subunits, T(3 3 7)/(2 2 5), is divided by a π chain with 1× periodicity. Two chain structures, H and π chains, commute with each other depending upon the external stresses perpendicular to the chain, which is the same for two row structures, D/A and T rows. It can be concluded that the wide and planar reconstruction of Si(5 5 12)-2 × 1 is originates from the stress balance among two commutable chains and two commutable rows.     

Anharmonicity in Al vicinal surfaces of (1 0 0) with (1 1 1) step

Molecular dynamics simulations incorporating an analytic embedded atom potential have been used to investigate the atomic structure and surface order of the Al vicinal surfaces for the temperature up to 900 K. The relaxation, mean square vibrational amplitude, and structure factor as a function of temperature, and of the terrace width for the p(1 0 0) × (1 1 1) surfaces (2 ≤ p ≤ 10) are discussed. The obtained structure factor indicates that the anharmonic effect reduces with increasing terrace widths. The decrease of surface energy with increasing terrace width also supports this conclusion.     

Reversible electromigration of thallium adatoms on the Si(1 1 1) surface

By means of low-energy electron diffraction (LEED), we found a reversible structural change of on thallium (Tl) adsorbed Si(1 1 1) surfaces by switching the polarity of applied DC voltage for heating the sample. It was shown in the literature that Tl adatoms are located on the T₄ sites of the bulk-terminated surface both in the (1 × 1) and . It is clarified that the structural change is caused by the electromigration of the Tl adatoms. Tl atoms migrate towards the cathode, being induced by the electric field (10-20 V/cm). We discussed an atomic process of the electromigration.