Theory of Isotope Effects on He+ Trapping in Solid Hydrogen

We are currently investigating the influence of vibrational effects on the strength of trapping of He⁺ in solid hydrogen. Such effects can lead to an isotope dependence of the trapping energy associated with the hydrogen molecules and He⁺ ion. At the present time, our focus is on the isotope effect for ³He⁺ and ⁴He⁺, which we are studying through the vibrational motions of the trapped He⁺ ions in the potential they experience as they move about their equilibrium positions. The potential governing the vibrations has been obtained from Hartree–Fock cluster calculations of the total energy of the cluster composed of the He⁺ ion and up to the third nearest neighbor hydrogen molecules as a function of the displacement of the He⁺ ion from its trapped position. The energy eigenvalues for the ground vibrational states of ³He⁺ and ⁴He⁺ in this potential come out as 1.29 and 0.96 meV, respectively, leading to corresponding reductions by these amounts in the binding energy of 8.6 eV for both ions without vibrational effects. The difference of these reductions can be considered as an isotope shift, its value for this case being 0.33 meV. From the analysis for these results, it is suggested that isotope shift effects for deuteron and triton in solid D–T would have the same order of magnitude. A procedure for more accurate investigations of the isotope shifts is discussed. This revised version was published online in August 2006 with corrections to the Cover Date.     

Theory for Relative Strengths of Trapping of He+ Ions in Solid, Liquid and Gaseous Hydrogen

The study of trapping of He⁺ ion in solid hydrogen is important both as a problem in solid state physics and also as an applied physics problem in the field of muon catalyzed fusion (μCF). In μCF, He⁺ ion acts as a trap for μ⁻, interrupting the chain reaction aspect of the catalytic role of μ⁻ in producing fusion of deuteron and triton and of triton and triton in solid hydrogen composed of ²H–³H and ³H–³H molecules, respectively. Using the Hartree–Fock procedure, combined with procedures for including many-body effects, as well as relaxation effects associated with the He⁺–H₂ distances and the adjustment of the H–H separation, we have investigated the trapping of He⁺ in gaseous and solid state environments. For the former, the environment of He⁺ is simulated by a single hydrogen molecule and for the solid by clusters appropriately chosen to represent the hexagonal close-packed structure. Our results for the gaseous state indicate that the trapping is rather strong with a binding energy of 8.5 eV, with almost equal binding energy in the linear and triangular configurations with respect to the H–H direction. For the solid, both the likely sites for He⁺ trapping, namely the tetrahedral and octahedral interstitial sites, are also found to provide deep traps (8.6 eV) of almost equal strength, independent of the orientations of the neighboring molecules, showing that the trapping is not influenced by the orientational disorder in the surrounding hydrogen molecules. Further, the influence of next nearest neighbor hydrogen molecules is found to enhance the trapping energy for He⁺ substantially, by 0.6 eV, with the incorporation of the third nearest neighbors having a much smaller added effect, demonstrating the convergence of our results with respect to the size of the cluster chosen to simulate the solid. The substantial influence on the He⁺ trapping energy found for the neighbors beyond the nearest ones provides an explanation of the greater accumulation of helium in the solid state of hydrogen in μCF experiments as compared to the liquid. Suggestions are made regarding the possible reasons for the almost negligible accumulation of helium in the liquid state. This revised version was published online in August 2006 with corrections to the Cover Date.     

The formation mechanism and the binding energy the body—centred regular tetrahedral structure of He5^＋

We propose the formation mechanism of the body-centred regular tetrahedral structure of the He5^ cluster,The total energy curve for this structure has been calculated by using a modified arrangement channel quantum mechanics method.The result shows that a minimal energy of -13.9106 a.u.occurs at a separation of 1.14a0 between the nucleus at the centre and nuclei at the apexes.Therefore we obtain the binding energy of 0.5202a .u.for this structure.This means that the He5^ cluster may be stable with a high binding energy in a body-centred regular tetrahedral structure.     

Mechanism of electron exchange between low energy He+ and solid surfaces

A general picture on the mechanism of electron exchange between low energy He⁺ ions and solid surfaces is proposed on the basis of experiments on three-dimensional angle resolving ion scattering spectroscopy in which not only He⁺ but neutral He is used as a projectile.     

Exit angle dependence of charge-state distribution of backscattered He ions

Exit angle and energy dependences of the charge-state distribution of backscattered He ions were investigated when 500 keV He⁺ ions were incident on SiO₂. The energy dependence of the He⁺ fraction was estimated by comparing the measured He⁺ spectra with the simulated spectra of He ions in all charge states at the exit angles of 5-25° with respect to the SiO₂ surface. We found that the He⁺ fraction is almost independent of the exit angle at energies higher than 250 keV and the observed energy dependence of the He⁺ fraction is in good agreement with that for the carbon-foil-transmission experiment. In the low energy region (<250 keV), however, the He⁺ fraction decreases as the exit angle decreases.     

High-resolution mass spectrometric study of pure helium droplets,and droplets doped with krypton

Mass spectra of doped and undoped helium droplets are presented. The high resolution of the time-of-flight spectrometer (m/Δm ≅ 5000) makes it possible to fully resolve small helium cluster ions from impurities and to unambiguously identify abundance anomalies in the size distribution of He _n ⁺. The yield of He₄ ⁺ shows the well-known enhancement relative to other small cluster ions when the expansion changes from sub- to supercritical, provided the electron energy exceeds a value of 40 ± 1 eV, the threshold for formation of electronically excited ions. Upon doping with krypton, pure Kr _n ⁺ cluster ions containing up to 41 Kr atoms are observed. The spectra exhibit abundance anomalies at 13, 16, 19, 22 & 23, 26 and 29, in agreement with spectra obtained by ionization of bare krypton clusters that are formed in neat supersonic beams. Mixed clusters He _m Kr⁺ indicate closure of a solvation shell at m = 12.     

Desorption of cluster ions from adsorbed methane under cryogenic condition by low-energy ion irradiation

We have investigated ion desorption from adsorbed methane following keV He⁺ ion irradiation. The thickness of the adsorbed layer was precisely controlled. For mono-layered methane, only monomer ions (CH_x⁺) were desorbed by 1 keV He⁺ ion irradiation. On the other hand, a large number of cluster ions (C_nH_x⁺) up to n = 20 were desorbed from multi-layered film. Among cluster ions, molecular ions with CC bonds were found, which indicates that chemical bonds are newly formed by ion irradiation. Based on the results for thickness dependences of the mass spectral patterns, it was elucidated that the monomer ions are desorbed from the top surface layer through single electron excitation. While the cluster ions are formed mainly in the inside of the layers along the nuclear track due to the high-density electronic excitation, which is produced by nuclear collision between incident He⁺ ions and frozen molecules.     

kinetic energy reflection from polycrystals bombarded with Ar+, Kr+, and Xe+ ions

When the surface of a solid is bombarded with ions a fraction of the primary energy is reemitted by ion reflection and sputtering. The contribution of ion reflection or sputtering to energy reflection is determined by the mass ratio of the bombarding ions to the target atoms.^1,2 In the case of light ions the contribution of reflected ions is dominant. Results for He⁺ and Ne⁺ bombardment were described in a previous paper.³ The present paper deals with results for Ar⁺, Kr⁺, and Xe⁺ bombardment of the same targets as investigated before.³ The energies of the mass selected bombarding ions range from 9 to 16 keV. The measurements were carried out by means of the thermic detector described in a separate paper.⁴ For the given mass ratios most of the reemitted energy is related to sputtering.     

Structure of negative impurity ions in liquid helium

The experimental mobilities of negative halogen (Cl^?, F^?, and I^?) and metal (Ba^? and Ga^?) impurity ions in superfluid ⁴He are close to each other and much lower than the mobilities of not only He⁺ ions but also electron bubbles. It has been shown that the formation of multiatomic complexes (clusters or bubbles) around ions is responsible for this low mobility. Although the mobilities are similar, the structures of the resulting complexes are qualitatively different in the cases of halogens and metals: solid clusters, which are similar to a well-studied cluster at the He⁺ ion, are formed near halogen ions, which exhibit high electron affinities, whereas metal ions are localized in bubbles, which are similar to electron bubbles. The temperature and pressure dependence of the mobility of these complexes is qualitatively different. Experiments in this area, most likely, performed with a wider variety of negative ions, would enhance the understanding of the structure of charged complexes in liquid helium.     

Preferential sputtering of TIC under keV Ar+ ion bombardment: Simultaneous sputtering-ISS measurement with He+ and Ar+ ions

The composition change of the outermost atom layer of TiC(110) under ion bombardment with 1.5–3 keV He⁺ and He⁺ + Ar⁺ ions has been measured by ion scattering spectroscopy with He⁺ ions at different sample temperatures. It has been found that the preferential sputtering of C atoms takes place for both the He⁺ and Ar⁺ ion bombardment, however the preferred sputtering is more pronounced for Ar⁺ ions than for He⁺ ions. The ion bombardment with He⁺ ions at elevated sample temperatures hardly results in any change in surface composition below ～800°C, while Ar⁺ ion bombardment results in C enrichment for elevated temperatures as reported so far.     

Observation of clusters in a sputtering ion source

This paper reports previously unpublished results which were obtained in 1966. We systematically investigated the dependence of cluster ion intensities on the bombarding gases He⁺, Ar⁺ and Xe⁺ (energies: 4 to 12 keV, current densities: 100 mA/cm²). Frequently, the observed structures in the relative cluster intensities were quite puzzling, e.g. for A1 and Si. Attempts to correlate these structures to crystal configurations failed, nor did any pattern develop from simple valency considerations alone. Initial ion energy distribution measurements from 0 to 1200 eV showed significant differences for atomic ions and cluster ions. This effect is used to reduce interference problems caused by cluster ion peaks in SIMS applied to trace analysis of solids. The results are discussed and compared with those of other investigators, also including cluster formation by vaporization and sparking. Extending known theoretical considerations may possibly afford a general understanding of the intensity structure. The formation and ejection mechanisms of clusters, however, remain unknown. Thermal effects to explain the latter are definitely discounted by the magnitude of the observed initial cluster energy (> 10 eV). Also discussed are two phenomena which demonstrate the presence of the bombarding gas in the surface.     

Sputtering yields for light ions as a function of angle of incidence

The sputtering yield of Ni, Mo, and Au have been measured at oblique angles of incidence for H⁺-, D⁺-, and⁴He⁺-ion irradiation in the energy region from 1 to 8 keV. The yields were determined from the weight loss of the targets. For Ni and Mo the dependence of the sputtering yield on the angle of incidence was found to be much stronger for H⁺- and D⁺-ion than for⁴He⁺-ion irradiation. In all cases the maximum in the yield was found at angles of incidence ϑ≧80°, where ϑ is the angle measured from the surface normal. Furthermore the ratio of the maximum yield to the yeild at normal incidence increases with increasing surface binding energy of the target material as well as with increasing ion energy in the energy region inveestigated. The results are discussed qualitatively in view of a model for the sputtering mechanism for light ions.     

Energy transfer to a copper surface by low energy noble gas ion bombardment

The energy transferred to a copper surface by bombardment with Xe⁺, Ar⁺, and He⁺ ions with kinetic energies in the range 100–4000 eV has been studied by our group in previous experiments. There were significant experimental uncertainties for that data at energies below about 200 eV. The present investigation overlaps the previous work, extends the energy range to 10 eV, and includes data for Ne⁺. Particular emphasis is placed on the energy range below 200eV. A specially designed ion source was employed in these experiments. A polycrystalline copper film deposited onto a highly sensitive calorimeter was used as the target material. The results show that the Xe⁺ ion deposits more than 97% of its energy over the entire range investigated whereas the lighter ions deposit a decreasing fraction of their energy below about 1 keV. The decrease is largest for the lightest ion (He⁺). In all cases the deposited energy is about or more than 70% of the incident energy. It will be shown that the present results are in agreement with previous measurements for copper and are qualitatively in good agreement with computer calculations using the TRIM.SP code.On leave from: Institut für Schicht- und Ionentechnik, Forschungszentrum Jülich GmbH, W-5170 Jülich, Fed. Rep. Germany     

Ion beam induced reaction of carbon films on Si(1 0 0)

The irradiation effects of 2 MeV He⁺ and Ar⁺ ions on the film structure of the C–Si system were investigated with RHEED and XPS. The formation of SiC phase and/or the growth of epitaxial SiC were possible by He⁺ irradiation for the carbon films up to 0.7 nm in thickness, which was thinner than that by Ar⁺ irradiation. The He⁺ irradiation could not grow the turbostratic graphite which could be grown by Ar⁺ irradiation. The mechanism of the formation and the epitaxial growth of SiC by ion irradiation was discussed from the view point of the energy transfer from the irradiated ions.     

Luminescent collisions of He+ and He++ ions with H2 molecules at energies below 2 keV

Spectroscopic studies of collisions between He⁺ and He⁺⁺ ions with H₂ gas target have been performed in the 200–600 nm wavelength range. Atomic lines of hydrogen Balmer series and several helium lines were identified and their excitation functions between 50 eV and 1 keV (2 keV for He⁺⁺) were determined.     

Surface analysis by ion-electron spectroscopy; Silicon target

The energy spectra of secondary elections emitted from a Si(111) surface due to bombardment by 6 keV He⁺ and O⁺₂ ions have been examined. The fine structure in the spectra is explained on the basis of a novel mechanism of creation of Auger electrons at the surface. There are two stages of interaction between incoming ions and the substrate via adsorbed atoms. In the first stage, due to a level promotion mechanism, vacancies in the adsorbed atoms are created. In the second stage, Auger neutralization processes accompanied by the emission of electrons from a solid with characteristic energies take place. These electrons provide a good indication of the degree of coverage of the silicon surface with contaminant atoms. The energy losses of escaping electrons are also discussed.     

A new observation method of ion-electron emission

The energy spectra of secondary electrons emitted from a molybdenum target in the shape of a wire upon bombardment with 5 keV He⁺ ions is examined. It is shown that for the grazing angleof ion incidence the structure of the energy spectrum is most sensitive to the target treatment. At such a geometry the ion-electron emission can be used for analysis of the solid surface covered by adsorbed or contaminant particles.     

Spectres auger et sections efficaces d'ionisation de la couche L23 du magnésium et de l'aluminium sous impact de protons et d'ions lourds (10–100 keV)

A comparison of Auger structures observed on the energy distributions of secondary electrons emitted from Mg and A1 solid targets bombarded by either light particles (H⁺ and He⁺) or heavy ions (Ne⁺, Ar⁺, …) is presented. With incident protons, it essentially appears a broad peak corresponding to a L₂₃VV transition and a weak shoulder due to the surface and bulk plasmon excitation. The Auger structures obtained with heavy ions are richer and the peaks which compose it are sharper. Such atomic-like structures correspond to Auger transitions from excited (with one or two L₂₃ holes) moving recoiling atoms. The experimental L₂₃ Mg and A1 ionization cross sections were determined from Auger spectra. In H⁺?Mg (or A1) collisions our results are in good agreement with the theoretical values calculated in a PWBA model. In the case of heavy ion-target interactions, we compared the experimental measurements with ionization cross section calculations obtained in a Landau-Zener model.     

Fragmentation of polyatomic ions produced by electron-loss collisions of butane and isobutane molecules with ions of kiloelectronvolt energy

Fragmentation accompanying the loss of electrons by butane and isobutane (C₄H₁₀) molecules in collisions with energy H⁺, He²⁺, and Ar⁶⁺ ions of kiloelectronvolt energies is studied. The electron density functional technique is applied to C _n H_2n+2 alkane molecules and their respective C _n H _2n+2 ⁺ ions to carry out quantum-chemical calculations of the atomic spacing, electron total energy for the initial configuration of the ionizing molecules and ions in the ground state, and atomic bond breaking energy necessary to produce different ion fragments. The fragmentation energy is correlated with the fragmentation probability. It is shown that the relative cross sections of ion fragmentation depend primarily on the related energy consumption. However, the process cross section is also strongly affected by the initial configuration of C₄H₁₀ isomer molecules, as well as by the amount of dangling and arising atomic bonds involved in the formation of each ion fragment.