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.     

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.     

Internal energy distribution of sputtered sulfur molecules

Bombarding targets of CS₂ and sulfur with keV Ar⁺ ions induces among other species the sputtering of S₂ molecules. We measured the internal energy (vibration and rotation) of these sputtered molecules with a laser induced fluorescence technique. The results show a Boltzmann behaviour for both the vibrational and rotational distributions. A vibrational temperature T_vib = 1500 K and a rotational temperature T_rot = 300 K is obtained for both target materials. The results are compared with different ejection mechanisms, where a molecule on the surface receives one (single collision) or two (double collision) momentum transfers from the solid. Two classical models are able to explain part of the experimentally observed internal energy distribution: a Monte Carlo calculation of the double collision model, and a single collision model assuming a sudden momentum transfer to the molecule as a whole, which yields an analytical expression (via a relation between the internal and kinetic energy). If we assume that some additional rotational cooling, due to time dependent relaxation effects, occurs during the ejection from the surface, the experimental results can be reasonably interpreted within the proposed sputtering models.     

Cluster-induced sputtering of molecular targets

Using molecular-dynamics simulation, we study the cluster-induced sputtering of a diatomic (O₂) and a triatomic (H₂O) molecular target and compare it to the sputtering of an atomic target (Ar). In all three systems, sputtering occurs by the flow of gasified material out of the spike volume into the vacuum above it. Above a threshold, the sputter yield and also the number of dissociations and reactions increase linearly with the total impact energy. The number of reactions occurring is significantly higher than the number of surviving dissociations. The degrees of freedom of the sputtered molecules are not in thermal equilibrium with each other. While for the diatomic target, the internal energy amounts to only 10-20% of the translational energy, it is 40% for H₂O. The translational energy distributions of sputtered monomers are strongly reduced at high energies due to molecule dissociations.     

The angular distribution of sputtered silver atoms

Angular distributions of sputtered atoms have been determined for a Ag target under bombardment with 20 and 30 keV ²⁰Ne⁺, ⁴⁰Ar⁺, ⁸⁴Kr⁺ and ¹³²Xe⁺ ions both at normal and oblique angles of incidence. At normal ion incidence the distribution is symmet with respect to the target normal, while at oblique ion incidence the distribution is asymmetric in the plane containing the ion beam and the surface normal and symmetric in the transverse plane. Scanning electron microscopy of the sputtered surface shows the development of a high density array of cones in the bombarded area. The results are discussed from the viewpoint of sputtering from a very rough surface.     

Dynamics of cluster induced sputtering in gold

Impacts of 0.13-1.4 MeV Au₁₃ clusters onto Au(1 1 1) target are investigated in molecular dynamics simulations. The evolution of sputtered Au atoms and clusters are simulated up to 10 ns. The total sputtering yield, angular and velocity distributions of the sputtered material, as well as dimensions of impact induced craters are compared to recent experimental results. It is shown that the experimental observations can be explained by a flow of atoms from the craters. Secondary cluster ejection from crowns formed around the craters is found to be one of the main mechanisms of sputtering. The results are summed up in an empirical model.     

Collision cascade temperature

Interaction of a projectile with a solid has been considered in detail. It has been found that any collision cascade generated by a projectile can be characterized by the average kinetic energy of cascade atoms that represents an “instantaneous temperature” of the cascade during its very short lifetime (10⁻¹² s). We refer to this value as the “dynamic temperature” in order to emphasize the fact that cascade atoms are in a dynamic equilibrium and have a definite energy distribution. The dynamic temperature defines the electron distribution in the cascade area and, hence, the ionization probability of sputtered atoms. The energy distribution of cascade atoms and, as a consequence, the dynamic temperature can be found experimentally by measuring the energy distribution of sputtered atoms. The calculated dynamic temperature has been found to be in good agreement with the experimental data on ion formation in the case of cesium and oxygen ion sputtering of silicon. Based on the developed model we suggest an experimental technique for a radical improvement of the existing cascade sputtering models.     

Determination of ion fraction and energy analysis of sputtered particles from deuterium bombarded surfaces

Ion energy distributions and sputtering yields have been measured in the presence of various background gases for deuterium, helium and argon ions in the 1–40 keV energy range. Alteration of the surface chemistry of hydride forming metals such as Ti, Y and V by exposure to hydrogen has a significant effect on the charge state of the sputtered particles. Under conditions likely to prevail in plasma devices and possible reactors, the ion/neutral fraction may be drastically increased, reaching ~41% for Ti. Such large ion fractions for metal targets have been previously observed only by sputtering with oxygen ions and present the possibility of improved impurity control in plasma devices. Both gas adsorption and recoil implantation are involved in the mechanism determining the ion fraction of sputtered products.     

Depth of origin of sputtered atoms for elemental targets

The mean depth of origin of sputtered atoms is an important characteristic of the sputtering process. There exist several theoretical and experimental determinations of the escape depth with different results. To clear up the situation, in the present work a systematic computer simulation study of the mean depth of origin of sputtered atoms is performed. The Monte Carlo program TRIM.SP and the lattice code OKSANA are applied to calculate the distribution of depth of origin and the dependences of the mean depth of origin on the atomic density, N, projectile energy, E, the angle of incidence, α, projectile and target atomic species, Z₁ and Z₂, as well as the simulation model.     

Cu－37at％ Ag共晶合金的离子溅射研究

侧重研究了入射Ａｒ＋离子不同剂量轰击时表面微形貌和溅射原子角分布之间的关联，并建议用“元素按靶点表面微形貌特征局域富集模型”来解释溅射原子角分布形状以及择优溅射曲线的变化；发现其结果与实验相符合。     

Electronic excitation in sputtered atoms and the oxygen effect

Bombardment of surfaces by ions gives rise to a variety of inelastic collision events leading to the ejection of excited atoms and ions. Such excited sputtered particles have been studied since more than 80 years through their optical emission, when they decay in front of the target to the electronic ground state, having lifetimes of 10⁻⁹ to 10⁻⁷ s, typically. Information on the energy distribution of such excited states can be obtained by two different techniques: light vs distance measurements (LvD) and by studying line profile broadening in light emission due to the Doppler effect. Only recently it has become possible to study in addition metastable excited atoms using laser induced fluorescence spectroscopy (LIF). Relative sputtering yields and energy distributions have been measured for such metastable states and two types can be distinguished. States with a very low excitation energy (0–0.3 eV), being sublevels of the electronic ground state, were found to have yields and energy distributions comparable to the electronic ground state, while metastable states at higher excitation energies (above 1 eV) seem to behave similar to short lived excited states, typically observed in secondary photon emission (BLE) with excitation energies in the range of 2–6 eV. This behaviour is also clearly visible with respect to oxygen surface coverage or increased near surface oxygen concentration where, similar to secondary ion emission, drastic changes in the yield by orders of magnitude have been found for excited atoms as well as for ions. In addition, under the same conditions a strong decrease in the sputtering yield of neutral ground state atoms has been observed for a number of metals. LIF results for highly excited metastable states are compared with recent results obtained by studying line profile broadening in light emission for Ca, Al and Cr targets. Different mechanisms that have been proposed to account for the observations will be discussed.     

Investigation of the projectile atomic number influence to the total sputtering yield in the keV energy region

The non-monotonous dependence of the total sputtering yield on the projectile atomic number, which is unexpected in the frame of the Sigmund linear cascade theory, is investigated using Monte Carlo simulations (program SRIM 2003). This effect is studied on the example of aluminum sputtering by six different projectiles (N, Ne, Al, Ar, Kr and Xe) at normal incidence. The incident projectile energy is 2 keV. Investigation consists of the analyses of ASI distributions of sputtered atoms as well as of nuclear energy loss depth distributions of projectiles with fixed number of ejected atoms. The results show that the non-monotonous behavior of Y(Z) is due to the ability of projectiles somewhat lighter than aluminum to efficiently eject large number of atoms by formation of collision cascades in the subsurface region which are directed towards the surface. On the other hand, ions that are heavier or significantly lighter than aluminum cannot form this type of cascades - the heavier ions cannot transfer a lot of energy to recoils in a primary knock-on collision that will move towards the surface, while significantly lighter ions transfer the energy too deep into the target.     

Energy distributions of neutral atoms sputtered by very low energy heavy ions

Polycrystalline Cu was sputtered by normally incident, very low energy Ar⁺ ions (E₀ = 40–1000 eV). The kinetic energy (E) distributions of the neutral Cu atoms sputtered normally from the Cu surface were measured, using secondary neutral mass spectrometry. For values of E₀ above approximately 600 eV, the observed energy distributions agreed closely with the Thompson-Sigmund theory. For values of E₀ less than about 600 eV the distributions fell off faster than predicted by the Thompson-Sigmund theory, and the peak value of the distribution shifted to somewhat lower energies. Both these effects were exaggerated as E₀ was further lowered. The average kinetic energy of the sputtered neutral Cu atoms increased with increasing E₀. The rate of this increase was less at higher values of E₀.     

Synergism in sputtering of copper nanoclusters on graphite substrate at low energy Cu2 bombardment

Molecular dynamics simulation of Cu cluster sputtering by 50-200 eV/atom Cu₂ dimers and Cu single atoms has been performed. The clusters were located on a (0 0 0 1) graphite surface and consisted of 13-195 atoms. Synergy features were identified in the sputtering yield and energy distributions of sputtered particles calculated for the cases of cluster bombardment with Cu dimers and monomers at the same velocity. The reason for the nonlinear effects in surface cluster sputtering is the overlapping of collision cascades generated by each of the dimer atoms.     

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.     

Erosion of methane induced by electron bombardment

Condensed layers of methane at 20 K. have been bombarded by electrons with an energy of 265 and 515 eV. The neutral sputtered flux was analyzed for mass and kinetic energy. Besides CH₄ also larger molecules are sputtered. During this process an involatile residue is formed. The kinetic energy distributions for methane, obtained from the times of flight, fit a Maxwell-Boltzmann distribution curve with T = 170 K. These results are explained by exothermic chemical processes which are initiated by the electrons and which lead to spots with a higher temperature. Large molecules which do not desorb are subjected to chemical reactions which ultimately lead to a nonvolatile residue.     

Angular distributions of Ni and Ti atoms sputtered from a NiTi alloy under He and Ar ion bombardment

The angular distributions of sputtered components were measured for NiTi polycrystalline alloy under 9 keV Ar⁺ and He⁺ ions bombardments with various fluences in ultrahigh vacuum. Combination of Rutherford Backscattering Spectrometry (RBS) and Auger Electron Spectrometry (AES) techniques allowed us to observe enhanced concentration of Ni over a layer with thickness comparable to a primary He⁺ ions penetration depth due to selective sputtering of Ti atoms and radiation-induced diffusion processes. A preferential emission of Ni atoms towards the surface normal was observed during bombardment by both He⁺ and Ar⁺ ions. More forward-peaked “over-cosine” angular distributions of sputtered Ni in comparison with those for Ti atoms have been measured. Nonstoichiometric sputtering of NiTi alloy dependent on emission angle was observed for bombardment fluence of He⁺ well below that needed for the steady-state altered layer formation. To explain the peculiarities of NiTi sputtering, an interpretation is discussed in terms of sputtering due to backscattered He⁺ ions.     

Modelling the erosion of beryllium carbide surfaces

Redeposition of beryllium eroded from main chamber plasma facing components of ITER onto the divertor material carbon creates a mixed material, beryllium carbide Be₂C, whose interaction with the plasma is not well known. In this study, we have investigated the erosion of Be₂C by deuterium using molecular dynamics simulations and ERO impurity modelling. We found that beryllium sputters preferentially over carbon and identified the sputtering mechanism in the ion energy range 10-100 eV to be both physical and swift chemical sputtering. In addition to single atoms, different types of small molecules/clusters were sputtered, the most frequently occurring molecules being BeD, Be₂D, and CD. The sputtering threshold was found to lie between 10 and 15 eV. The MD sputtering yields were used in plasma impurity simulations, serving as a replacement for input data obtained with TRIM. This changes the accumulation rate of impurity Be in the divertor region compared to previous estimates.     

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.