First-Principles Calculations of Atomic and Electronic Properties of T1 and In on Si（111）

The atomic and electronic structures of T1 and In on Si（111） surfaces are investigated using the firstprinciples total energy calculations. Total energy optimizations show that the energetically favored structure is 1/3 ML T1 adsorbed at the T4 sites on Si（111） surfaces. The adsorption energy difference of one T1 adatom between （√3 × √3） and （1 × 1） is less than that of each In adatom. The DOS indicates that TI 6p and Si 3p electrons play a very important role in the formation of the surface states. It is concluded that the bonding of TI adatoms on Si（111） surfaces is mainly polar covalent, which is weaker than that of In on Si（111）. So T1 atom is more easy to be migrated than In atom in the same external electric field and the structures of T1 on Si（111） is prone to switch between （√3 × √3） and （1 × 1）.     

Ar adsorptions on Al （111） and Ir （111） surfaces： a first-principles study

We investigate the adsorptions of Ar on Al (111) and Ir (111) surfaces at the four high symmetry sites,i.e.,top,bridge,fcc-and hcp-hollow sites at the coverage of 0.25 monolayer (ML) using the density functional theory within the generalized gradient approximation of Perdew,Burke and Ernzerhof functions.The geometric structures,the binding energies,the electronic properties of argon atoms adsorbed on Al (111) and Ir (111) surfaces,the difference in electron density between on the Al (111) surface and on the Ir (111) surface and the total density of states are calculated.Our studies indicate that the most stable adsorption site of Ar on the Al (111) surface is found to be the fcc-hollow site for the (2 × 2) structure.The corresponding binding energy of an argon atom at this site is 0.538 eV/Ar atom at a coverage of 0.25 ML.For the Ar adsorption on Ir (111) surface at the same coverage,the most favourable site is the hcp-hollow site,with a corresponding binding energy of 0.493 eV.The total density of states (TDOS) is analysed for Ar adsorption on Al (111) surface and it is concluded that the adsorption behaviour is dominated by the interaction between 3s,3p orbits of Ar atom and the 3p orbit of the base Al metal and the formation of sp hybrid orbital.For Ar adsorption on Ir (111) surface,the conclusion is that the main interaction in the process of Ar adsorption on Ir (111) surface comes from the 3s and 3p orbits of argon atom and 5d orbit of Ir atom.     

First-principle study of Mg adsorption on Si（111） surfaces

We have carried out first-principle calculations of Mg adsorption on Si(111) surfaces. Different adsorption sites and coverage effects have been considered. We found that the threefold hollow adsorption is energy-favoured in each coverage considered, while for the clean Si(111) surface of metallic feature, we found that 0.25 and 0.5 ML Mg adsorption leads to a semiconducting surface. The results for the electronic behaviour suggest a polarized covalent bonding between the Mg adatom and Si(111) surface.     

Modifying Quantum Well States of Pb Thin Films via Interface Engineering

We demonstrate the importance of interface modification on improving electron confinement by preparing Pb quantum islands on Si（111） substrates with two different surface reconstructions, i.e., Si（111）-7 ×7 and Si（111）- Root3×Root3-Pb （hereafter, 7 ×7 and R3）. Characterization with scanning tunneling microscopy/spectroscopy shows that growing Pb films directly on a 7 × 7 surface will generate many interface defects, which makes the lifetime of quantum well states （QWSs） strongly dependent on surface locations. On the other hand, QWSs in Pb films on an R3 surface are well defined with small variations in linewidth on different surface locations and are much sharper than those on the 7 × 7 surface. We show that the enhancement in quantum confinement is primarily due to the reduced electron-defect scattering at the interface.     

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.     

Initial Processes of Hydrogen Adsorption on Si（100） Surface

The adsorption of one monolayer H atoms on an ideal Si(100) surface is studied by using the self-consistent tight binding linear muffin-tin orbital method. Energies of adsorption systems of H atoms on different sites are calculated.It is found that the adsorbed H atoms are more favorable on B1 site (bridge site) with a distance 0.056 nm above the Si surface. There does not exist reaction barrier at the Si surface. The layer projected density states are calculated and compared with those of the clean surface. The charge transfers are also investigated.     

First-principles study of Ar adsorptions on the （111） surfaces of Pd, Pt, Cu, and Rh

In the present paper we give a detailed report on the results of our first-principles investigations of Ar adsorptions at the four high symmetry sites on M （111） （M =Pd, Pt, Cu, and Rh） surfaces. Our studies indicate that the most stable adsorption sites of Ar on Pd （111） and Pt （111） surfaces are found to be the fcc-hollow sites. However, for Ar adsorptions on Cu （111） and Rh （111） surfaces, the most favorable site is the on-top site. The density of states （DOS） is analyzed for Ar adsorption on M （111） surfaces, and it is concluded that the adsorption behavior is dominated by the interaction between 3s, 3p orbits of Ar atoms and the d orbit of the base metal atoms.     

Chemisorption of Au on Si（001） surface

The chemisorption of one monolayer of Au atoms on an ideal Si(001) surface is studied by using the self-consistent tight binding linear muffin-tin orbital method. Energies of the adsorption system of a Au atom on different sites are calculated. It is found that the most stable position is A site (top site) for the adsorbed Au atoms above the Si(001) surface. It is possible for the adsorbed Au atoms to sit below the Si(001) surface at the B_1 site(bridge site), resulting in a Au－Si mixed layer. This is in agreement with the experiment results. The layer projected density of states is calculated and compared with that of the clean surface. The charge transfer is also investigated.     

Initial Processes of Sulfur Adsorption on Si（100） Surface

The adsorption of one monolayer S atoms on ideal Si（100） surface is studied by using the self-consistent tight binding linear muffon-tin orbital method. Energies of adsorption systems ors atoms on different sites are calculated. It is found that the adsorbed S atoms are more favorable on B1 site （bridge site） with a distance 0.131 nm above the Si surface. The .S, Si mixed layer might exist at S/Si（100） interface. The layer projected density of states are calculated and compared with that of the clean surface. The charge transfers are also investigated.     

Chemisorption of Fe on Au-passivated Si（001） surface

The chemisorption of one monolayer of Fe atoms on a Au-passivated Si(001) surface is studied by using the self-consistent tight-binding linear muffin-tin orbital method. The Fe adatom chemisorption on an ideal Si(001) surface is also considered for comparison. The chemisorption energy and layer projected density of states for a monolayer of Fe atoms on Au-passivated Si(001) surface are calculated and compared with that of the Fe atoms on an ideal Si(001) surface. The charge transfer is investigated. It is found that the most stable position is at the fourfold hollow site for the adsorbed Fe atoms, which might sit below the Au surface. Therefore there will be a Au－Fe mixed layer at the Fe/Au－Si(100) interface. It is found that the adsorbed Fe atoms cannot sit below the Si surface, indicating that a buffer layer of Au atoms may hinder the intermixing of Fe atoms and Si atoms at the Fe/Au－Si(001) interface effectively, which is in agreement with the experimental results.     

Influence of Pb adatom on adsorption of oxygen molecules on Pb(111) surface: a first-principles study

Using first-principles calculations, we systematically study the influence of Pb adatom on the adsorption and the dissociation of oxygen molecules on Pb(111) surface, to explore the effect of a point defect on the oxidation of the Pb(111) surface. We find that when an oxygen molecule is adsorbed near an adatom on the Pb surface, the molecule will be dissociated without any obvious barriers, and the dissociated O atoms bond with both the adatom and the surface Pb atoms. The adsorption energy in this situation is much larger than that on a clean Pb surface. Besides, for an adsorbed oxygen molecule on a clean Pb surface, a diffusing Pb adatom can also change its adsorption state and enlarge the adsorption energy for O, but it does not make the oxygen molecule dissociated. And in this situation, there is a molecule-like PbO2 cluster formed on the Pb surface.     

A density-functional theory investigation on desorption of O2 on Sn（111） and its comparison with initial oxidation on the X（111） （X=Si,Ge, Sn,Pb） surfaces

<正>The first-principles calculations are performed to investigate the adsorption of O₂ molecules on an Sn（111） 2×2 surface.The chemisorbed adsorption precursor states for O₂ are identified to be along the parallel and vertical channels, and the surface reconstructions of Sn（lll） induced by oxygen adsorption are studied.Based on this,the adsorption behaviours of O₂ on X（111）（X=Si,Ge,Sn,Pb） surfaces are analysed,and the most stable adsorption channels of O₂ on X（111）（X=Si,Ge,Sn,Pb） are identified.The surface reconstructions and electron distributions along the most stable adsorption channels are discussed and compared.The results show that the O₂ adsorption ability declines gradually and the amount of charge transferred decreases with the enhancement of metallicity.     

Tunable Adsorption and Desorption of Hydrogen Atoms on Single-Walled Carbon Nanotubes

Chemical adsorption and desorption of hydrogen atoms on single-walled carbon nanotubes(SWNTs) are investigated by using molecular dynamics simulations.It is found that the adsorption and desorption energy of hydrogen atoms depend on the hydrogen coverage and the diameter of the SWNTs.Hydrogen-adsorption geometry at the coverage of 1.0 is more energetically stable.The adsorption energy decreases with the increasing diameter of the armchair tubes.The adsorption and desorption energy of hydrogen atoms can be modified reversibly by externally radial deformation.The averaged C-H bond energy on the high curvature sites of the deformed tube increases with increasing radial deformation,while that on the low curvature sites decreases.     

Atomic Diffusion in Cu/Si （111） and Cu/SiO2/Si （111） Systems by Neutral Cluster Beam Deposition

The Cu films are deposited on two kinds of p-type Si （111） substrates by ionized duster beam （ICB） technique. The interface reaction and atomic diffusion of Cu/Si （111） and Cu/SiO2/Si （111） systems are studied at different annealing temperatures by x-ray diffraction （XRD） and Rutherford backscattering spectrometry （RBS）. Some significant results are obtained： For the Cu/Si （111） samples prepared by neutral dusters, the interdiffusion of Cu and Si atoms occurs when annealed at 230℃. The diffusion coefficients of the samples annealed at 230℃ and 500℃ are 8.5 ×10^-15 cm^2.s^-1 and 3.0 ×10^-14 cm^2.s^-1, respectively. The formation of the copper-silicide phase is observed by XRD, and its intensity becomes stronger with the increase of annealing temperature. For the Cu/SiO2//Si （111） samples prepared by neutral dusters, the interdiffusion of Cu and Si atoms occurs and copper silicides are formed when annealed at 450℃. The diffusion coefficients of Cu in Si are calculated to be 6.0 ×10^-16 cm^2.s^-1 at 450℃, due to the fact that the existence of the SiO2 layer suppresses the interdiffusion of Cu and Si.     

Effects of rapid thermal annealing on the morphology and optical property of ultrathin InSb film deposited on SiO2/Si substrate

Ultrathin InSb films on SiO2/Si substrates are prepared by radio frequency(RF) magnetron sputtering and rapid thermal annealing(RTA) at 300,400,and 500℃,respectively.X-ray diffraction(XRD) indicates that InSb film treated by RTA at 500℃,which is higher than its melting temperature(about 485℃),shows a monocrystalline-like feature.A high-resolution transmission electron microscopy(HRTEM) micrograph shows that melt recrystallization of InSb film on SiO2/Si(111) substrate is along the(111) planes.The transmittances of InSb films decrease and the optical band gaps redshift from 0.24 eV to 0.19 eV with annealing temperature increasing from 300℃ to 500℃,which is indicated by Fourier transform infrared spectroscopy(FTIR) measurement.The observed changes demonstrate that RTA is a viable technique for improving characteristics of InSb films,especially the melt-recrystallized film treated by RTA at 500℃.     

Dissociations of O2 molecules on ultrathin Pb（111） films： first-principles plane wave calculations

Using first-principles calculations,we systematically study the dissociations of O₂ molecules on different ultrathin Pb（111） films.According to our previous work revealing the molecular adsorption precursor states for O₂,we further explore why there are two nearly degenerate adsorption states on Pb（111） ultrathin films,but no precursor adsorption states existing at all on Mg（0001） and Al（111） surfaces.The reason is concluded to be the different surface electronic structures.For the O₂ dissociation,we consider both the reaction channels from gas-like and molecularly adsorbed O₂ molecules.We find that the energy barrier for O₂ dissociation from the molecular adsorption precursor states is always smaller than that from O₂ gas.The most energetically favorable dissociation process is found to be the same on different Pb（111） films,and the energy barriers are found to be influenced by the quantum size effects of Pb（111） films.     

Origin of the metallic to insulating transition of an epitaxial Bi(111) film grown on Si(111)

Transport characteristics of single crystal bismuth films on Si(111)-7×7 are found to be metallic or insulating at temperatures below or above T_C, respectively. The transition temperature T_C decreases as the film thickness increases. By combining thickness dependence of the films resistivity, we find the insulating behaviour results from the states inside film, while the metallic behaviour originates from the interface states. We show that quantum size effect in a Bi film, such as the semimetal-to-semiconductor transition, is only observable at a temperature higher than T_C.     

Comparative study of adsorption characteristics of Cs on the GaN(0001) and GaN(000) surfaces

The adsorption characteristics of Cs on GaN(0001) and GaN(000) surfaces with a coverage from 1/4 to 1 monolayer have been investigated using the density functional theory with a plane-wave ultrasoft pseudopotential method based on first-principles calculations.The results show that the most stable position of the Cs adatom on the GaN(0001) surface is at the N-bridge site for 1/4 monolayer coverage.As the coverage of Cs atoms at the N-bridge site is increased,the adsorption energy reduces.As the Cs atoms achieve saturation,the adsorption is no longer stable when the coverage is 3/4 monolayer.The work function achieves its minimum value when the Cs adatom coverage is 2/4 monolayer,and then rises with Cs atomic coverage.The most stable position of Cs adatoms on the GaN(000) surface is at H3 site for 1/4 monolayer coverage.As the Cs atomic coverage at H3 site is increased,the adsorption energy reduces,and the adsorption is still stable when the Cs adatom coverage is 1 monolayer.The work function reduces persistently,and does not rise with the increase of Cs coverage.     

Coadsorption of gold with chlorine on CeO2 (111) surfaces: A first principles study

To investigate the effects of chlorine on the Au/ceria catalysts,the adsorption of gold or chlorine and their coadsorpiton on the stoichiometric and partially reduced CeO₂（111） surfaces are studied from the first principles.It is found that the adsorption of Au is significantly enhanced by the chlorine preadsorption on the stoichiometric CeO₂（111） surface;while on the partially reduced CeO₂（111） surface,the preadsorbed chlorine inhabits the oxygen vacancy（which is the preferred adsorption site for gold）,leading to a CeOCl phase and the dramatical weakening of the Au adsorption.Therefore,chlorine on the CeO₂（111） surface can affect the Au adsorption thus the activity of the Au/CeO₂ catalyst.     

Methane adsorption on graphite（0001） films： A first-principles study

Using first-principles methods, we have systematically investigated the electronic density of states, work function, and adsorption energy of the methane molecule adsorbed on graphite(0001) films. The surface energy and the interlayer relaxation of the clean graphite(0001) as a function of the thickness of the film were also studied. The results show that the interlayer relaxation is small due to the weak interaction between the neighboring layers. The one-fold top site is found most favourable on substrate for methane with the adsorption energy of 133 meV. For the adsorption with different adsorption heights above the graphite film with four layers, the methane is found to prefer to appear at about 3.21 A above the graphite. We also noted that the adsorption energy does not dependent much on the thickness of the graphite films. The work function is enhanced slightly by adsorption of methane due to the slight charge transfer from the graphite surface to the methane molecule.