Dependence of cluster ranges on target cohesive energy: Molecular-dynamics study of energetic Au402 cluster impacts

It has long been known that the stopping and ranges of atoms and clusters depends on the projectile-target atom mass ratio. Recently, Carroll et al. [S.J. Carroll, P.D. Nellist, R.E. Palmer, S. Hobday, R. Smith, Phys. Rev. Lett. 84 (2000) 2654] proposed that the stopping of clusters also depends on the cohesive energy of the target. We investigate this dependence using a series of molecular-dynamics simulations, in which we systematically change the target cohesive energy, while keeping all other parameters fixed. We focus on the specific case of Au₄₀₂ cluster impact on van-der-Waals bonded targets. As target, we employ Lennard-Jones materials based on the parameters of Ar, but for which we vary the cohesive energy artificially up to a factor of 20. We show that for small impact energies, E₀ ? 100 eV/atom, the range D depends on the target cohesive energy U, D ∝ U^−β. The exponent β increases with decreasing projectile energy and assumes values up to β = 0.25 for E₀ = 10 eV/atom. For higher impact energies, the cluster range becomes independent of the target cohesive energy. These results have their origin in the so-called ‘clearing-the way’ effect of the heavy Au₄₀₂ cluster; this effect is strongly reduced for E₀ ? 100 eV/atom when projectile fragmentation sets in, and the fragments are stopped independently of each other. These results are relevant for studies of cluster stopping and ranges in soft matter.     

Alkali ion scattering from Ag(0 0 1) and Ag thin films at low and hyperthermal energies

We have investigated the scattering of K⁺ and Cs⁺ ions from a single crystal Ag(0 0 1) surface and from a Ag-Si(1 0 0) Schottky diode structure. For the K⁺ ions, incident energies of 25 eV to 1 keV were used to obtain energy-resolved spectra of scattered ions at θ_i = θ_f = 45°. These results are compared to the classical trajectory simulation safari and show features indicative of light atom-surface scattering where sequential binary collisions can describe the observed energy loss spectra. Energy-resolved spectra obtained for Cs⁺ ions at incident energies of 75 eV and 200 eV also show features consistent with binary collisions. However, for this heavy atom-surface scattering system, the dominant trajectory type involves at least two surface atoms, as large angular deflections are not classically allowed for any single scattering event. In addition, a significant deviation from the classical double-collision prediction is observed for incident energies around 100 eV, and molecular dynamics studies are proposed to investigate the role of collective lattice effects. Data are also presented for the scattering of K⁺ ions from a Schottky diode structure, which is a prototype device for the development of active targets to probe energy loss at a surface.     

Improved calculation of Si sputter yield via first principles derived interatomic potential

Silicon sputter yield under medium energy Ar+ ion bombardment is calculated via molecular dynamics, using a highly accurate interatomic potential for Ar-Si interactions derived from first-principles calculations. Unlike the widely used universal repulsive potentials such as the Moliere or ZBL parameterizations, this new potential, referred to as DFT-ArSi, is developed via localized basis density functional theory. Sputter yields for Si obtained with the DFT-ArSi potential at 500 eV and 1 keV incident energies are found to be within 6% and 2% of experimental results, respectively, while errors using existing potentials are typically on the order of 11%. The DFT-ArSi potential differs from existing empirical potentials in the ∼1 Å interatomic separation range which is shown to be the most important range for modeling low-to-medium energy ion bombardment.     

Growth and surface morphology of ion-beam sputtered Ti-Ni thin films

Titanium-nickel thin films have been deposited on float glass substrates by ion beam sputtering in 100% pure argon atmosphere. Sputtering is predominant at energy region of incident ions, 1000 eV to 100 keV. The as-deposited films were investigated by X-ray photoelectron spectroscopy (XPS) and atomic force microscope (AFM). In this paper we attempted to study the surface morphology and elemental composition through AFM and XPS, respectively. Core level as well as valence band spectra of ion-beam sputtered Ti-Ni thin films at various Ar gas rates (5, 7 and 12 sccm) show that the thin film deposited at 3 sccm possess two distinct peaks at binding energies 458.55 eV and 464.36 eV mainly due to TiO₂. Upon increasing Ar rate oxidation of Ti-Ni is reduced and the Ti-2p peaks begin approaching those of pure elemental Ti. Here Ti-2p peaks are observed at binding energy positions of 454.7 eV and 460.5 eV. AFM results show that the average grain size and roughness decrease, upon increasing Ar gas rate, from 2.90 μm to 0.096 μm and from 16.285 nm to 1.169 nm, respectively.     

Cesium/xenon co-sputtering at different energies during ToF-SIMS depth profiling

In this paper, ToF-SIMS dual beam depth profiles of H-terminated silicon wafers were performed with cesium primary ions and for different beam energies. The aim of this study was to investigate the influence of the cesium beam energy on the secondary ion yields during ToF-SIMS dual beam depth profiling. For this purpose, both the cesium beam energy and the cesium surface concentration were varied but the analysis conditions were kept identical for all depth profiles (i.e. Ga⁺ at 25 keV, 45°). For each sputter beam energy (i.e. 250 eV, 750 eV and 2000 eV), the cesium surface concentration was varied by diluting the cesium sputtering beam by xenon ions. This technique allows performing ToF-SIMS depth profiles with cesium surface concentration varying from zero (for pure xenon beam) to a maximum value (for pure Cs beam), depending on the bombardment conditions. For all the beam energies, the Si⁺ signals were found to decrease with the increasing cesium coverage and the lower the energy, the faster the decrease. The Cs⁺, the SiCs⁺ and the signals were found to exhibit a maximum for well defined Cs/Xe mixtures, which were found to depend on the secondary ion species and on the beam energy. Moreover, the maxima were found to shift to higher Cs beam content with the increasing energy. This effect is due to the variation of the cesium surface concentration with the varying beam energy. XPS analysis of the Cs/Xe craters and DYNTRIM computer simulations allowed us to convert the cesium beam scale to a cesium surface concentration scale and to interpret our results.     

Electronic stopping power of hydrogen in KCl at the stopping maximum and at very low energies

The electronic energy loss of hydrogen ions in KCl was investigated in a wide energy range. Thin films of KCl were evaporated on an Au/Si substrate. Rutherford Backscattering Spectrometry (RBS) was performed with protons and deuterons at energies from 30 to 400 keV/nucleon. At lower energies experiments were performed by Time-Of-Flight Low energy ion scattering (TOF-LEIS) again with proton and deuteron projectiles. Experimental results are compared to calculated/tabulated values for the electronic energy loss. Whereas at energies beyond the stopping maximum very good agreement is found, at lower ion energies discrepancies between experiment and calculations increase. At very low ion velocities the extrapolated stopping cross section ε predicts vanishing electronic energy loss at energies below 100 eV/nucleon.     

On the emission of MoCs molecular ions from Cs irradiated molybdenum surface

The present paper deals with the emission of atomic and molecular ions from elemental molybdenum surface under Cs⁺ bombardment to explore the MCs⁺ formation mechanism with changing Cs surface coverage. Integrated count of MoCs⁺ shows a monotonic increase with increasing primary ion energy (1-5 keV). Change in MoCs⁺ intensity is attributed to the variation of surface work function ? and cesium surface concentration c_Cs due to varying impact energies. Variation of c_Cs has been obtained from the expression, c_Cs ∝ 1/(1 + Y) where Y is the elemental sputtering yield estimated from TRIM calculations. Systematic study of the energy distributions of all species emerging from Mo target has been done to measure the changes in surface work function. Changing slopes of the leading parts of Cs⁺ energy distributions suggest a substantial depletion in surface work function ? with decreasing primary ion energies. Δ? shows a linear dependence on c_Cs. The maximum reduction in surface work function Δ?_max = 0.69 eV corresponds to the highest value of c_Cs = 0.5. A phenomenological model, based on the linear dependence of ? on c_Cs, has been employed to explain the MoCs⁺ data.     

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.     

Resonant Auger decay of 2p hole in argon induced by electron impact

We present an experimental study of L-MM resonant Auger spectra of argon after electron impact excitation. The electron spectra were measured at ten different electron impact energies between 442.6 eV and 461.7 eV. During (e, 2e) measurement the energy of the second electron was kept fixed at 209.6 eV, corresponding to the energy of one of the strongest resonant Auger transitions from the [2p_3/23d] state. Except for the monopole excitations, the recorded spectral structures are explained on the basis of photon impact data.     

Monte Carlo study of ion-induced backward and forward secondary electron emission from thin Al foil

A direct Monte Carlo program has been developed to calculate the backward (γ_b) and forward (γ_f) electron emission yields from 20 nm thick Al foil for impact of C⁺, Al⁺, Ar⁺, Cu⁺ and Kr⁺ ions having energies in the range of 0.1-10 keV/amu. The program incorporates the excitation of target electrons by projectile ions, recoiling target atoms and fast primary electrons. The program can be used to calculate the electron yields, distribution of electron excitation points in the target and other physical parameters of the emitted electrons. The calculated backward electron emission yield and the Meckbach factor R = γ_f/γ_b are compared with the available experimental data, and a good agreement is found. In addition, the effect of projectile energy and mass on the longitudinal and lateral distribution of the excitation points of the electrons emitted from front and back of Al target has been investigated.     

Molecular simulations of cluster ejection by CO2 cluster impact on carbon-based surfaces

Single (CO₂)_N (N = 1-20) cluster impact on three different carbon-based surfaces of fullerite (1 1 1), graphite and diamond (1 0 0) has been investigated by MD simulations with the cluster collision energy from 5 to 14 keV/cluster as a first step toward the general modeling of the reactive sputtering by cluster impact of a solid surface. A crater permanently remained on the fullerite and graphite surfaces while it was quickly replenished with fluidized carbon material on the diamond surface. In spite of the smaller crater size as well as the crater recovery resulting in the reduction of the surface area, the sputtering yields were the highest on diamond. The effective energy deposition near the surface contributes to the temperature rise and consequent sputtering seemed highly reduced due to the collision cascades especially on the fullerite target.     

Competition of terrace and step-edge sputtering under oblique-incidence ion impact on a stepped Pt(1 1 1) surface

Using molecular-dynamics simulation, we study the sputtering of a Pt(1 1 1) surface under oblique and glancing incidence 5 keV Ar ions. For incidence angles larger than a critical angle ?_c, the projectile is reflected off the surface and the sputter yield is zero. We discuss the azimuth dependence of the critical angle ?_c with the help of the surface corrugation felt by the impinging ion. If a step exists on the surface, sputtering occurs also for glancing incidence ?>?_c. We demonstrate that for realistic step densities, the total sputtering of a stepped surface may be sizable even at glancing incidence.     

Calculated depth-dose distributions for H and He beams in liquid water

We have calculated the dose distribution delivered by proton and helium beams in liquid water as a function of the target-depth, for incident energies in the range 0.5-10 MeV/u. The motion of the projectiles through the stopping medium is simulated by a code that combines Monte Carlo and a finite differences algorithm to consider the electronic stopping power, evaluated in the dielectric framework, and the multiple nuclear scattering with the target nuclei. Changes in projectile charge-state are taken into account dynamically as it moves through the target. We use the MELF-GOS model to describe the energy loss function of liquid water, obtaining a value of 79.4 eV for its mean excitation energy. Our calculated stopping powers and depth-dose distributions are compared with those obtained using other methods to describe the energy loss function of liquid water, such as the extended Drude and the Penn models, as well as with the prediction of the SRIM code and the tables of ICRU.     

Monte Carlo study of ion-induced secondary electron emission from SiO2

Here we describe a recently developed direct Monte Carlo program to study kinetic electron emission from SiO₂ target. The program includes excitation of the target electrons (by projectile ions, recoiling target atoms and fast primary electrons), subsequent transport and escape of these electrons from the target surface. The program can be used to calculate the electron yields, distribution of electron excitation points in the target and other physical parameters of the emitted electrons. In order to demonstrate the capabilities of this program, we report a study on the kinetic electron emission from SiO₂ induced by fast (1-10 keV) rare gas ions. The calculated kinetic electron yield for various ion energies and masses is in good agreement with the predictions of most frequently applied theoretical model. In addition, the effects of projectile energy, mass and impact angle on the depth distribution of electron excitation points and average escape depth of the outgoing electrons were investigated. It is important to mention that the existing experimental techniques are not capable to measure these parameters.     

Ion guiding in alumina capillaries: MCP images of the transmitted ions

Transmission of a few keV impact energy Ne⁶⁺ ions through capillaries in anodic alumina membranes has been studied with different ion counting methods using an energy dispersive electrostatic spectrometer, a multichannel plate (MCP) array and sensitive current-measurement. In the present work, we focus our attention to the measurements with the MCP array. The alumina capillaries were prepared by electro-chemical oxidation of aluminium foils. For the present experiments guiding of 3-6 keV Ne⁶⁺ ions has been studied in two samples with capillary diameter of about 140 nm and 260 nm and with capillary length of about 15 μm. At these energies, the ions have been efficiently guided by the capillaries up to few degrees tilt angle. In this work, we compare the results obtained by the energy dispersive spectrometer to those studied by the MCP array.     

First-principles study on electronic structures of BaMoO4 crystals containing F and F color centers

The electronic structures of perfect crystals of barium molybdate (BaMoO₄) and of crystals containing F and F⁺ color centers are studied within the framework of the fully relativistic self-consistent Dirac-Slater theory by using the numerically discrete variational (DV-Xα) method. The calculated results suggest that the donor energy level of the F center as well as F⁺ center is located within the band gap. The respective optical transition energies are 1.86 eV and 2.105 eV corresponding to the wavelength of the absorption band of 668 nm and 590 nm. It is therefore suggested that these bands are originate from the F and F⁺ centers in the crystal.     

Proton sputtering from polycrystalline Al surface interacting with highly charged ions at grazing incidence angle

Sputtering processes of protons from a polycrystalline Al surface interacting with Ar^q+ (q = 3-14) ions at a grazing incidence angle (∼0.5°) were investigated. The intensity of protons (I_H) detected in coincidence with scattered Ar atoms was measured as a function of q. I_H saturated at q ? 10, although it increased rapidly with q at 3 ? q ? 8. The angular distribution of protons with low kinetic energy (?2 eV) began to deviate from the cosine distribution and assumed a rather flat equidistribution as q increased. To analyze the sputtering processes of protons at the grazing incidence angle, a modified model of the “above-surface potential sputtering model” was proposed by considering image acceleration of projectile ions.     

Predicting the probability for fission gas resolution into uranium dioxide

Classical molecular dynamics simulations, using a set of previously established pair potentials, have been used to predict the minimum energy needed for krypton and xenon atoms to be resolved into uranium dioxide across a perfect (1 1 1) surface. The absolute minimum energy, E_min, is 53 eV for krypton and 56 eV for xenon atoms, significantly less than the 300 eV value often assumed in fuel modelling as the minimum energy required for gas resolution. The present values are, however, still sufficient to preclude thermal resolution at normal reactor temperatures. The discrepancies between the present and previous resolution energies are due to the significant variation in probabilities of absorption at different impact points on the crystal surface; we have mapped out the probability distribution for various impact sites across the crystal surface. The value of 300 eV corresponds to an 85% chance of resolution.     

Desorption of gold nanoclusters from gold nanodispersed targets by 200 keV Au5 polyatomic ions in the elastic stopping mode: Experiment and molecular-dynamics simulation

Au nanoislet targets (∅ 2-60 nm) were bombarded by 200 keV polyatomic ions (40 keV/atom), which deposit their energy mainly in the nuclear stopping mode: ∑(dE/dx)_n = 30 keV/nm and ∑(dE/dx)_e = 2 keV/nm. The matter desorbed in the form of nanoclusters was registered by TEM. The total transfer of matter was determined by neutron-activation analysis. The total yield of the ejected gold reached high values of up to 2.6 × 10⁴ atoms per Au₅ ion. The major part (2 × 10⁴ atoms per ion Au₅) of the emission is in the form of nanoclusters. The results are compared with the data of similar experiments with 1 MeV Au₅ (200 keV/atom) and other projectiles. The analysis of the experimental data and the comparison to molecular-dynamics simulation results of the desorption process show that the desorption of Au nanoislets is induced by their melting, build-up of pressure and thermal expansion.