Proximity-Effect-Induced Anisotropic Superconductivity in a Monolayer Ni-Pb Binary Alloy.

A proximity effect facilitates the penetration of Cooper pairs that permits superconductivity in a normal metal, offering a promising approach to turn heterogeneous materials into superconductors and develop exceptional quantum phenomena. Here, we have systematically investigated proximity-induced anisotropic superconductivity in a monolayer Ni-Pb binary alloy by combining scanning tunneling microscopy/spectroscopy (STM/STS) with theoretical calculations. By means of high-temperature growth, the (33×33)R30o Ni-Pb surface alloy has been fabricated on Pb(111) and the appearance of a domain boundary as well as a structural phase transition can be deduced from a half-unit-cell lattice displacement. Given the high spatial and energy resolution, tunneling conductance (dI/dU) spectra have resolved the reduced but anisotropic superconducting gap ΔNiPb ≈ 1.0 meV, in stark contrast to the isotropic ΔPb ≈ 1.3 meV. In addition, the higher density of states at the Fermi energy (D(EF)) of the Ni-Pb surface alloy results in an enhancement of coherence peak height. According to the same Tc ≈ 7.1 K with Pb(111) from the temperature-dependent ΔNiPb and the short decay length Ld ≈ 3.55 nm from the spatially monotonic decrease of ΔNiPb, both results are supportive of a proximity-induced superconductivity. Despite a lack of a bulk counterpart, the atomically thick Ni-Pb bimetallic compound opens a pathway to engineer superconducting properties down to the two-dimensional limit, giving rise to the emergence of anisotropic superconductivity via a proximity effect.

How dissociated fragments of multiatomic molecules saturate all active surface sites-H2O adsorption on the Si(100) surface.

A fundamental question for the adsorption of any gas molecule on surfaces is its saturation coverage, whose value can provide a comprehensive examination for the adsorption mechanisms, dynamic and kinetic processes involved in the adsorption processes. This investigation utilizes scanning tunneling microscopy to visualize the H2O adsorption processes on the Si(100) surface with a sub-monolayers (<0.05 ML) of chemically-reactive dangling bonds remaining after exposure to (1) a hydrogen atomic beam, (2) H2O, and (3) Cl2gases at room temperature. In all three cases, each of the remaining isolated single dangling bonds (sDB) adsorb and is passivated by either of the two dissociation fragments, the H or OH radical, to form a surface Si-H and Si-OH species. A new adsorption mechanism, termed 'dissociative and asynchronous chemisorption', is proposed for the observation presented herein. Upon approaching a sDB site, the H2O molecule breaks apart into two fragments. One is chemisorbed to the sDB. The other attaches to the same or the neighboring passivated dimer to form a transition state of surface diffusion, which then diffuses on the mostly passivated surface and is eventually chemisorbed to another reactive site. In other words, the chemisorption reactions of the two fragments after dissociation occur at different and uncorrelated time and places. This adsorption mechanism suggests that a diffusion transition state can be an adsorption product in the first step of the dissociative adsorption processes.

Controlling the Polarity of the Molecular Beam Epitaxy Grown In-Bi Atomic Film on the Si(111) Surface.

Synchrotron radiation core-level photoemission spectroscopy, scanning tunneling microscopy (STM), and first-principles calculations have been utilized to explore the growth processes and the atomic structure of the resulting films during the two-step molecular beam epitaxy (MBE) of In and Bi on the Si(111) surface. Deposition of 1.0-ML Bi on the In/Si(111)-(4 × 1) surface at room temperature results in Bi-terminated BiIn-(4 × 3) structures, which are stable up to ~300 °C annealing. By contrast, deposition of In on the ß-Bi/Si(111)-(√3 × âˆš3) surface at room temperature results in three dimensional (3D) In islands. In both cases, annealing at 460 °C results in the same In-terminated In0.75Bi/Si(111)-(2 × 2) surface. Our DFT calculations confirm that the surface energy of In-terminated In0.75Bi/Si(111)-(2 × 2) system is lower than that of Bi-terminated Bi0.75In/Si(111)-(2 × 2). These findings provide means for the control of the polarity of the MBE In-Bi atomically thick films.

Ordered 2D Structure Formed upon the Molecular Beam Epitaxy Growth of Ge on the Silicene/Ag(111) Surface.

Growth of Ge by molecular beam epitaxy (MBE) on top of the silicene monolayer on the Ag(111) surface results in either a dispersed adlayer or a two-dimensional (2D) ordered structure depending on the silicene phase. Scanning tunneling microscopy (STM) images show that the ordered adsorbed Ge atoms on (3 × 3)Si domains occupy a position directly on top of down atoms in the buckled silicene layer, similar to the adatom positions on the Ge(111)-c(2 × 8) surface. By contrast, no long-range ordering of Ge adatoms is observed on the domain, possibly partly because of the interference effects of the Ag substrate. Results herein suggest that the deposited Ge atoms tend to build an additional three-dimensional bulk layer on the silicene monolayer and that the growth of the 2D germanene/silicene heterostructure may not be achieved in a straightforward manner.

Gold atomic clusters extracting the valence electrons to shield the carbon monoxide passivation on near-monolayer core-shell nanocatalysts in methanol oxidation reactions.

Atomic-scale gold clusters were intercalated at the inter-facet corner sites of Pt-shell Ru-core nanocatalysts with near-monolayer shell thickness. We demonstrated that these unique clusters could serve as a drain of valence electrons in the kink region of the core-shell heterojunction. As jointly revealed by density functional theory calculations and valence band spectra, these Au clusters extract core-level electrons to the valence band. They prevent corrosion due to protonation and enhance the tolerance of CO by increasing the electronegativity at the outermost surface of the NCs during the methanol oxidation reaction (MOR). In these circumstances, the retained current density of Pt-shell Ru-core NCs is doubled in a long-term (2 hours) MOR at a fixed voltage (0.5 V vs. SCE) by intercalating these sub-nanometer gold clusters. Such novel structural confinement provides a possible strategy for developing direct-methanol fuel cell (DMFC) modules with high power and stability.

Hard repulsive barrier in hot adatom motion during dissociative adsorption of oxygen on Ag(100).

Random pairing simulation and low temperature scanning tunneling microscopy (STM) are used to investigate the detailed O(2) dissociative adsorption processes at 200 K for various coverages. The distribution of oxygen adatoms shows a strong repulsion between the adsorbates with a radius of approximately 0.8 nm. The comparison between STM results and simulation reveals two prominent pairing distances of 2 and 4 nm and their branching ratio is about 2:1. These findings shed new light on the origin of the large intrapair distances found and on the process behind the empirical "eight-site rule."

Ion segregation and deliquescence of alkali halide nanocrystals on SiO2.

The adsorption of water on alkali halide (KBr, KCl, KF, NaCl) nanocrystals on SiO2 and their deliquescence was investigated as a function of relative humidity (RH) from 8% to near saturation by scanning polarization force microscopy. At low humidity, water adsorption solvates ions at the surface of the crystals and increases their mobility. This results in a large increase in the dielectric constant, which is manifested in an increase in the electrostatic force and in an increase in the apparent height of the nanocrystals. Above 58% RH, the diffusion of ions leads to Ostwald ripening, where larger nanocrystals grow at the expense of the smaller ones. At the deliquescence point, droplets were formed. For KBr, KCl, and NaCl, the droplets exhibit a negative surface potential relative to the surrounding region, which is indicative of the preferential segregation of anions to the air/solution interface.

Mediation of chain reactions by propagating radicals during halogenation of H-masked Si(100): implications for atomic-scale lithography and processing.

Scanning tunneling microscopy reveals a free radical-induced surface chain reaction in the chlorination of nanoscale patterns on an otherwise H-passivated (masked) Si(100). While scanning probe methods can be used to pattern active surface regions with single-bond precision, follow-up selective chemical vapor deposition with polyatomic molecules can produce various filling characteristics. On active surface regions, molecular Cl(2) undergoes an atom abstraction reaction in which a Si dangling bond abstracts one atom of the incident Cl(2) molecule while the complementary Cl atom is scattered away from the initial abstraction site either back into the vacuum or to be captured by a second dangling bond and adsorbed there, or to react with a nearby adsorbed H atom to form volatile HCl. In contrast, I(2) undergoes only dissociative adsorption on two immediately neighboring dangling bonds, whereby two I-Si bonds are formed simultaneously upon cleavage of the I(2) bond. The different chemisorption processes of the two model diatomic molecular gases place intrinsic limitations on atomic-scale lithography and processing: Adsorption of Cl(2) results in spillage over the prepatterned regions of active bonds. In contrast, adsorption of I(2) is a pair process and results in under-filling.

Correlation of reaction sites during the chlorine extraction by hydrogen atom from ClSi(100)-2x1.

The Cl abstraction by gas-phase H atoms from a Cl-terminated Si(100) surface was investigated by scanning tunneling microscopy (STM), high-resolution core level photoemission spectroscopy, and computer simulation. The core level measurements indicate that some additional reactions occur besides the removal of Cl. The STM images show that the Cl-extracted sites disperse randomly in the initial phase of the reaction, but form small clusters as more Cl is removed, indicating a correlation between Cl-extracted sites. These results suggest that the hot-atom process may occur during the atom-adatom collision.