Low-energy ion scattering and sputtering at grazing ion bombardment of clean and oxygen covered Ag(1 1 0) surface

The ion scattering and sputtering processes at low energy grazing N⁺ and Ne⁺ ion bombardment of clean and oxygen covered Ag(1 1 0) surface have been investigated by computer simulation in the binary collision approximation.

The spatial, angular and energy distributions of scattered, sputtered particles and desorbed molecules of oxygen as well as their yields versus the angle of incidence have been calculated. In these distributions the some characteristic peaks were observed and analysed. It was found that an adsorption layer plays a role of the additional surface barrier, i.e. it reflects leaving target atoms back to crystal. The azimuth angular dependencies of Ag sputtering yield and non-dissociative O₂ desorption yield at grazing incidence have been calculated. It was shown that these dependencies correlate the crystal orientation.     

Cluster size effect on reactive sputtering by fluorine cluster impact using molecular dynamics simulation

The mechanism of high-yield sputtering induced by reactive cluster impact was investigated using molecular dynamics (MD) simulations. Various sizes of fluorine clusters were radiated on clean silicon surface. At an incident energy of 1 eV/atom, F atom and F₂ molecule are only adsorbed on the surface and sputtering of Si atom does not occur. However, fluorine cluster, which consists of more than several tens molecules causes sputtering. In this case, most of Si atoms are sputtered as fluorinated material such as SiF_x. This effect is due to the fact that cluster impact induces high-density particle and energy deposition, which enhances both formation of precursors and desorption of etching products. The deposition of atoms and energy becomes denser as the incident cluster size increases, so that larger clusters have shown higher sputtering yield.     

Sputtering of thin benzene films by large noble gas clusters

Molecular dynamics computer simulations have been employed to investigate the sputtering process of a benzene (C₆H₆) monolayer deposited on Ag{1 1 1} induced by an impact of slow clusters composed of large number of noble gas atoms. The sputtering yield, surface modifications, and the kinetic energy distributions of ejected species have been analyzed as a function of the cluster size and the binding energy of benzene to the Ag substrate. It is shown that high- and low-energy components can be identified in the kinetic energy distributions of ejected molecules. The mechanistic analysis of calculated trajectories reveals that high-energy molecules are emitted by direct interaction with projectile atoms that are backreflected from the metal substrate. Most of the molecules are ejected by this process. Low-energy molecules are predominantly emitted by a recovering action of the substrate deformed by the impact of a massive cluster. The increase of the binding energy leads to attenuation of both high- and low-energy ejection channels. However, low-energy ejection is particularly sensitive to the variation of this parameter. The area of the molecular overlayer sputtered by the projectile impact is large and increases with the cluster size and the kinetic energy of the projectile. Also the size and the shape of this area are sensitive to the changes of the binding energy. The radius of the sputtered region decreases, and its shape changes from almost circular to a ring-like zone when the binding energy is increased. Some predictions about the perspectives of the application of large clusters in the organic secondary ion mass spectrometry are discussed.     

Desorption of large organic molecules induced by keV projectiles

In order to understand the emission of organic molecules in sputtering, classical molecular dynamics (MD) is used to model the 5 keV Ar atom bombardment of polystyrene oligomers adsorbed on Ag{1 1 1}. The analysis of the results shows that a significant fraction of the trajectories generates high action events in the sample. These events are characterized by the simultaneous motion of several hundreds of substrate atoms and, oftentimes, by high emission yields of substrate atoms, clusters and polystyrene molecules. Collision trees representing the energetic part of the cascades confirm that high sputtering yields of molecules occur when a large portion of the primary particle energy is quickly dissipated in the upper layers of the silver substrate. This class of events where high action occurs in the surface region might explain the ejection of organic species with a mass of several kilodaltons such as biomolecules and synthetic polymers. In the simulation, these events are capable of desorbing polystyrene molecules of 2 kDa.     

Temporal development of sputtered atom distributions from Au(1 1 1) targets following bombardment with 100 keV/atom Au2 ions

Recently Bouneau et al. measured the angular and energy distributions of negative Au_n (n=2–7) ions emitted from gold targets following bombardment with swift gold cluster projectiles. They found that the energy distributions could be fitted with a spike-like model, and that the angular distributions were independent of the azimuthal emission angle and relatively strongly forward directed. We have used MD simulations to investigate the temporal development of energy and angular distributions of sputtered atoms from Au(1 1 1) targets following bombardment with 100 keV/atom Au₂ ions. Our results show that during the very early stages of the collision cascade the energy distribution of sputtered atoms is described well by the linear cascade model. Essentially all high energy sputtered atoms are emitted during this phase of the collision cascade. However, the energy distributions of atoms sputtered after 0.5 ps were typical of emission from a thermal spike and could be fitted well with a Sigmund–Claussen model. The polar angle distributions of sputtered atoms were strongly forward directed early in the collision cascade, but became less forward directed as the thermal spike developed.     

He scattering on a TiO2(1 1 0) surface

We present measurements of energy-losses and neutralisation of helium ions on a TiO₂(1 1 0) surface at low keV energies. Measurements were performed in the 1–4 keV energy range. The target azimuthal orientation dependence of total scattering intensity profiles, energy-losses and probability of electron capture or loss were determined. On the basis of Marlowe simulations it is concluded that ion scattering intensities give indications about defects regarding surface bridging O atoms. Variations in energy losses for different scattering directions are reported. Ion fraction measurements were made using both incident ions and neutrals. Similar ion fractions were found indicating that He is efficiently neutralised and ions result from reionisation. These ion fractions are found to depend on the azimuthal orientation and have a minimum along the main crystallographic directions.     

Investigation of cascade-induced re-solution from nanometer sized coherent precipitates in dilute Fe–Cu alloys

Molecular dynamics (MD) simulations have been used to investigate the re-solution of copper atoms from coherent, nanometer-sized copper precipitates in a body-centered cubic iron matrix. The molecular dynamics simulations used Finnis–Sinclair type interatomic potentials to describe the Fe–Cu system. Precipitate diameters of 1, 3 and 5 nm were studied, with primary knock-on atom (PKA) from 1 to 100 keV, although the majority of the cascade simulations and analysis of solute re-solution were performed for cascades of 10 or 20 keV. The simulation results provide an assessment of the re-solution on a per-atom basis as a function of precipitate size, cascade location and energy. Smaller sized precipitates, with a larger surface to volume ratio, experienced larger re-solution on a per-atom basis than larger precipitates. Re-solution was observed to occur predominantly in the initial ballistic stages of the cascades when atomic collisions occur at high kinetic energy. A minimum PKA energy of around 1 keV was required to produce re-solution, and the amount of re-solution appears to saturate for PKA energies above approximately 10 keV, indicating that the MD results are representative of the energy range of interest. A model for prompt, cascade induced solute atom re-solution has been derived, following the approach used to describe fission gas bubble re-solution, and the parameters for describing copper atom re-solution are provided.     

Mixed resolution model for C60 cluster bombardment of solid benzene

Molecular dynamics simulations of C₆₀ cluster bombardment have been instrumental in elucidating physical phenomena related to the sputtering process; however, chemical phenomena can also play an important role in C₆₀ cluster bombardment of molecular solids. Therefore, a mixed resolution model of C₆₀ cluster bombardment is being developed, where the reactive zone is represented by an all atom region, and the remaining part of the target is described by a coarse-grained representation. A reactive many body potential describes the interactions among atoms; whereas, pair potentials describe the interactions between coarse-grained beads and between coarse-grained beads and atoms. Solid benzene is used to develop the methodology of blending the potentials. The blending of potentials is evaluated by the differences in the velocities of the pressure waves (generated by the C₆₀ impact) between the all atom benzene, coarse-grained benzene and the mixed resolution benzene systems. Initial testing with 1 keV C₆₀ cluster bombardment simulations show a smooth transition between regions.     

Neutralization of keV Ne and Ar ions during grazing scattering from an Al(1 1 1) surface

Charge fractions after scattering of Ne⁺ ions, Ne⁰ atoms and Ar⁺ ions with keV energies under a grazing angle of incidence from an atomically clean and flat Al(1 1 1) surface are studied. For incoming Ne⁺ ions we observe defined ion fractions in the scattered beams, whereas for incident Ne⁰ atoms ion fractions are more than one order of magnitude smaller. This experimental result provides clear evidence for a survival of Ne⁺ ions over the whole scattering event. From the dependence of ion fractions on the perpendicular energy component we derive neutralization rates as function of distance from the surface. These rates compare well with recent theoretical calculations for the system He⁺–Al(1 1 1). For incident Ar⁺ ions no survival of ions is found and upper limits for the survival probability and lower limits for the neutralization rate are determined.     

Emission of large molecules from methane by ion bombardment

Condensed layers ot methane at 20 K have been bombarded by 6–8 keV Ar⁺, He⁺ and H₂⁺ ions. Mass spectra and Kinetic energy distributions of neutral species sputtered from these layers have been measured. We have found sputtered species with masses up to 72 amu and thus with at least 5 carbon atoms. In addition to this an involatile residue was formed. Analysis by pyrolysis mass spectrometry showed this residue to contain species with masses up to at least 170 amu which therefore contain at least 12 carbon atoms. The kinetic energy distributions of sputtered methane molecules lie between those of a Maxwell-Boltzmann distribution and a collision cascade. Higher values are reached for Ar⁺ than for the light ions. From these observations we conclude: for both light and heavy ions radicals are formed, which combine to new molecules. These exothermic reactions produce heat which causes desorption. The high energy tail for bombardment with argon ions shows that part of the sputtering is caused by momentum transfer.     

稀有气体原子与Pu（100）表面相互作用的第一性原理研究

采用第一性原理研究了稀有气体原子在Pu（100）表面上的吸附。计算结果表明：除He原子外,其他稀有气体原子在桥位处的吸附能均为最大;稀有气体原子在Pu（100）表面吸附后,稀有气体原子失去电荷,而Pu原子得到电荷,稀有气体原子中Xe原子的电荷转移数最大。差分电荷密度的计算结果表明,对位于Pu（100）表面穴位和桥位处的Xe原子,可观察到较明显的电荷再分布现象,这表明Xe原子具有一定极化效应,能与Pu（100）表面发生相互作用,从He到Xe,原子的极化效应越来越明显。     

Mechanism of adatom formation on Ag(1 1 0) studied by combined quasi-elastic He atom scattering and low energy ion scattering

Two complementary techniques, i.e. low-energy ion scattering in the neutral impact collision ion scattering spectroscopy (NICISS) mode and energy resolved He atom scattering (HAS) are combined to study the adatom formation mechanism on Ag(1 1 0). The NICISS spectra have been collected between 300 and 900 K along the 0 0 1, and azimuthal directions while HAS measurements of the diffuse elastic peak has been performed along the directions between 190 and 800 K. Both techniques are sensitive to surface disorder and HAS data have been corrected by using the NICISS results in particular on the anharmonicity estimated through a two atoms scattering model. In fact, above 500 K surface anharmonicity is clearly detected and accompanies the proliferation of thermal induced defects. Without this anharmonic correction the adatom formation energy E_a is too low and similar to the surface diffusion barrier. Instead, including the anharmonicity the estimate, E_a = (0.38 ± 0.03) eV, is in excellent agreement with the predictions of molecular dynamics simulations.     

Angular dispersion of protons passing through thin metallic films

The angular distributions of protons after traversing thin polycrystalline Al targets (15 nm) with an incident energy of 10 keV have been measured and an analysis of the targets by means of transmission electron microscopy (TEM) techniques has been made. The separate influence of the different crystal characteristics and defects has been evaluated by numerical simulation considering the interaction of the ion with all the nearest neighboring atoms simultaneously. In the analysis we included the evaluation of the effects of lattice vibrations, oxide layers and foil roughness on the angular distributions. Previous experimental data in monocrystalline and polycrystalline Au targets has also been analyzed. For a consistency check a comparison with the results of the MARLOWE code for the simpler case of proton channeling in 1 0 0 Al has been performed. As in the case of Au, the present results indicate that the experiments can be explained in terms of a modified Moliere potential, and confirm the critical influence of crystal characteristics, in this case the amorphous oxide layer on the surface and the thermal vibration of the lattice atoms.     

Dynamical simulations of radiation damage induced by 10 keV energetic recoils in UO2

We have performed classical molecular dynamics simulations to simulate the primary damage state induced by 10 keV energetic recoils in UO₂. The numbers versus time and the distance distributions for the displaced uranium and oxygen atoms were investigated with the energetic recoils accelerated along four different directions. The simulations suggest that the direction of the primary knock-on atom (PKA) has no effect on the final primary damage state. In addition, it was found that atomic displacement events consisted of replacement collision sequences in addition to the production of Frenkel pairs. The spatial distribution of defects introduced by 10 keV collision cascades was also presented and the results were similar to that of energetic recoils with lower energy.     

Preferential damage at symmetrical tilt grain boundaries in bcc iron

The interaction of collision cascades with a (5 3 0) symmetrical tilt grain boundary in bcc iron has been studied using molecular dynamics simulations. Collision cascades were generated by a principle knock-on atom PKA of 1 keV at various distances from the boundary and with different velocity directions. Simulations reflect how the grain boundary acts as a barrier and also as a region where defects can be easily conducted along the boundary plane. Results show that there exist preferential sites in the periodic structure of the (5 3 0) symmetrical tilt boundary where defects are formed. These sites have been identified together with the atomic rearrangements produced in the grain boundary atomic structure have been analysed. The grain boundary energy increases after radiation. This increase in energy is proportional to the number of defects inside the grain boundary region.     

Displacement cascade simulation of LiAlO2 using molecular dynamics

To elucidate the radiation damage process on an atomic scale, displacement cascade simulations of LiAlO₂ were performed using molecular dynamics. Results of simulations obtained when an oxygen atom as the primary knock-on atom was displaced with the energy of 1-5 keV showed that the correlation between migration barriers of point defects and the declining rate of the maximum kinetic energy of atom in the system determined the thermal spike duration. The thermal spike of each element might finish when the maximum kinetic energy among all atoms of each element diminishes at around the point defects’ migration barrier. Defect-cluster analysis revealed that vacancies produce larger clusters than interstitials do, perhaps because the strong Coulomb interaction in ionic materials renders interstitials resistant to aggregation.     

Sputtering from spherical Au clusters by energetic atom bombardment

Using molecular-dynamics simulation, we study the effect of 100 keV Au atom bombardment of spherical Au clusters (radius R=40 Å), containing 15,784 atoms. Results range from projectile transmission with only few atoms sputtered to more or less complete cluster disintegration. During disintegration, besides major fragments of the original cluster, monatomics and a large number of clusters with sizes up to 100 atoms, and even beyond, are created. Angular and energy spectra of sputtered atoms show features of both collisional sputtering and evaporation: particle emission is isotropic with an additional contribution of preferential emission along [1 1 0] directions. Energy spectra show the high-energy E⁻² fall-off typical of linear-cascade sputtering plus an additional low-energy thermal component.     

Surface morphology of the Ar ion-irradiated Ag/Si(1 1 1) system

In the present study, a 500 Å thin Ag film was deposited by thermal evaporation on 5% HF etched Si(1 1 1) substrate at a chamber pressure of 8×10⁻⁶ mbar. The films were irradiated with 100 keV Ar⁺ ions at room temperature (RT) and at elevated temperatures to a fluence of 1×10¹⁶ cm⁻² at a flux of 5.55×10¹² ions/cm²/s. Surface morphology of the Ar ion-irradiated Ag/Si(1 1 1) system was investigated using scanning electron microscopy (SEM). A percolation network pattern was observed when the film was irradiated at 200°C and 400°C. The fractal dimension of the percolated pattern was higher in the sample irradiated at 400°C compared to the one irradiated at 200°C. The percolation network is still observed in the film thermally annealed at 600°C with and without prior ion irradiation. The fractal dimension of the percolated pattern in the sample annealed at 600°C was lower than in the sample post-annealed (irradiated and then annealed) at 600°C. All these observations are explained in terms of self-diffusion of Ag atoms on the Si(1 1 1) substrate, inter-diffusion of Ag and Si and phase formations in Ag and Si due to Ar ion irradiation.