Latent track structure in polymers as observed by a highly sensitive electrolytical conductivity measurement

Abstract

First results of a new electrolytical conductivity cell are reported concerning the initial stage of the pore opening process during track etching in vitreous solids. On the basis of the soft mode (low-energy excitation) model for track etching, a distribution function for the number of perforated micropores as function of time is calculated by accounting for the radial etch rate as function of the effective pore radius.     

Track structure in dielectric and semiconductor single crystals irradiated by heavy ions with high level of inelastic energy losses

The phenomenological model of the track formation processes during a heavy ion passing through materials is discussed. This model is based on the scanning tunneling and electronic microscopy investigations of diamond single crystals and stainless steel subjected to ⁴⁰Ar, ⁸⁴Kr and ¹²⁹Xe ion irradiation with energies in the MeV region. The energy and temperature criteria when crater formation on the surface during the heavy ion irradiation takes place are introduced.     

FT-IR spectroscopy of carbon dioxide in CR-39 and SR-90 track detectors irradiated with ions and gamma-rays at different energies and fluences

Two types of polymeric track detectors CR-39 and SR-90 were irradiated with protons, alpha particles, heavy ions and gamma-rays at different energies and fluences. After irradiation these detectors were analyzed with an FT-IR spectrometer of Jasco type 5300 in transmission and ATR modes. We have found that CO₂ is produced not only by irradiation but also by polymerization. The amount of CO₂ in the detector material is closely related to the latent track formation.     

Optimization of the heavy nuclei track etching in olivine crystals from meteorites

The investigation of the track etching velocity dependence for nuclei with Z50 on pH of the etching solution in the olivine crystals from Marjalahti and Eagle Station meteorites, containing galactic cosmic-ray nuclear tracks and also the crystals from Marjalahti meteorite, calibrated at the UNILAC (GSI, Darmstadt) with 14.17 MeV/N ²⁰⁸Pb nuclei, were performed.

The pH of the etching solution were changed from 7.8 to 9.4. It is shown that the optimal track etch condition were realised at pH of etching solution in the interval from 8.4 to 8.8.

The results of the Galactic cosmic-ray nuclei tracks with Z83 revealed in olivine crystals are presented. They were additionally irradiated at 90% to the surface with accelerated 14 MeV/N ¹³²Xe nuclei.     

Coupled chemical reactions in dynamic nanometric confinement: IV. Ion transmission spectrometric analysis of nanofluidic behavior and membrane formation during track etching in polymers

In recent papers, it was shown that coupled chemical-topological reactions (CCRs) with both NaOH etchant and silver salts, performed in thin swift-heavy ion-irradiated polymers under the application of a test voltage across the polymer foils, eventually gave rise to characteristic current/voltage features and Bode plots that were tentatively attributed to the formation of Ag₂O membranes within the etched tracks. The same was also found when replacing the silver ions by lithium ions, and adding fluoride ions to the NaOH etchant, to promote LiF membrane formation. Ion Transmission Spectrometry (ITS) enabled us to reconfirm the existence of these membranes beyond doubt. The membrane thickness was determined to be ～0.2–0.4?µm in the best cases.

ITS also revealed that hitherto membrane formation occurs only in ～1% of all tracks, or even less. The reason for this poor abundance seems to be that the decisive factor for membrane formation, which is the firm anchoring of the emerging solid Ag₂O or LiF reaction products on the etched track walls, was hitherto rarely fulfilled. We attribute this tentatively to the too high test voltage applied for controlling the CCR process that might hinder the product anchoring on the walls by promoting nanofluidic electromigration. Indeed, voltage reduction seems to improve the situation.     

Comparison of Makrofol-E and CR-39 as Solid State Nuclear Track Detectors

A comparison of the etching parameters as well as the neutron response for Makrofol-E and CR-39 was considered as solid state nuclear track detectors. The calculated sensitivity for both detectors was compared with the measured one. It is found that CR-39 has higher response to fast neutrons than Makrofol-E. The response increase due to decreasing the rate of layer removed and increasing the etch-pits per unit area.     

Studies on the track formation mechanism of the heavy ions in CR-39

The bulk etch rate for two types of CR-39 detector was measured as a function of temperature and the activation energies of bulk etching was determined. Experimental values of track etch rate were derived directly from the function of the succesive measured track length vrs. etching time for ²⁰⁹Bi, ¹²⁹Xe and ²⁰Ne ions.

The maximum etchable length of 13 MeV/u ²⁰⁹Bi and 13.04 MeV/u ¹²⁹Xe ions have been measured at and below these energies. A comparison of the measured and calculated track length data is presented.     

Raman spectrum study of graphite irradiated by swift heavy ions

Highly oriented pyrolytic graphites are irradiated with 40.5-Me V and 67.7-Me V ^112Sn-ions in a wide range of fluences： 1×10^11 ions/cm^2–1×10^14ions/cm^2. Raman spectra in the region between 1200 cm^-1 and 3500cm^-1 show that the disorder induced by Sn-ions increases with ion fluence increasing. However, for the same fluence, the amount of disorder is greater for 40.5-Me V Sn-ions than that observed for 67.7-Me V Sn-ions, even though the latter has a slightly higher value for electronic energy loss. This is explained by the ion velocity effect. Importantly, ～ 3-cm^-1frequency shift toward lower wavenumber for the D band and ～ 6-cm^-1 shift toward lower wavenumber for the 2D band are observed at a fluence of 1×10^14 ions/cm^2, which is consistent with the scenario of radiation-induced strain. The strain formation is interpreted in the context of inelastic thermal spike model, and the change of the 2D band shape at high ion fluence is explained by the accumulation of stacking faults of the graphene layers activated by radiation-induced strain around ion tracks. Moreover,the hexagonal structure around the ion tracks is observed by scanning tunneling microscopy, which confirms that the strains near the ion tracks locally cause electronic decoupling of neighboring graphene layers.     

Thermal spike analysis of latent track information in magnetic insulators

A new thermal spike model is presented which predicts three regimes in the formation of latent tracks. At S_eS_et no track formation is expected. A logarithmic and a linear variation of the damage cross section versus S_e is predicted for 2.7S_etS_eS_et and S_eS_et, respectively. A simple expression is derived for the relation between S_et and the thermal properties of the target. A comparison is made with experimental data on YIG and NiFe₂O₄ and a good agreement is found.     

Distribution of lithium in doped nuclear pores of polyethylene terephthalate by neutron depth profiling

In this paper, doping of porous polyethylene terephthalate membrane using Li-based solution is described and analyzed by nuclear analytic methods. In recent years, the polymeric porous membranes have been studied as advanced battery separators in various applications, such as portable electronic devices or electric vehicles. Apart from mechanical stability, the separators also provide electrical separation and ionic transport between the electrodes during charging and discharging processes. For application of the membranes, it is important to follow the Li distribution in the separator material over time. In this work, the distribution of Li in the porous PET foils, adepts for Li ion battery separators, was analyzed by Neutron Depth Profiling and the 3D shape of the etched pores by Ion Transmission Spectroscopy. The data obtained show that Li can be incorporated, in a passive way in the micropores in large quantities, but its amount is still limited and does not depend on time of doping. Here, the first data are presented.     

XRD and AFM study of radiation damage induced by swift heavy ions in Y3Al5O12 single crystals

Defects induced in Y₃Al₅O₁₂ single crystals by swift heavy ions are investigated by X-ray diffraction (XRD) and atomic force microscopy. The irradiation was performed at GANIL with 561 MeV ⁵¹Cr, 466 MeV ¹²⁸Te, and 957 MeV ²⁰⁸Pb ions. The XRD data reveal that the lattice strain increases with increasing electronic stopping power, whereas the hillock parameters (height and diameter) are not influenced by the electronic stopping power. According to our experimental data, for the same mean electronic stopping power, the hillock parameters are more pronounced for the lower range in contrast to swelling measurements. The experimental data show a strong increase in the hillock parameter at higher fluence, indicating the amorphization of Y₃Al₅O₁₂ single crystals.     

Interaction of MEV atomic ions with molecular solids: Ion track structure and sputtering phenomena

Recent results obtained in our research groups from studies of the interactions of swift, heavy atomic ions with molecular solids are concisely outlined. The focus is on material ejection (sputtering) and surface track formation. The experimental techniques employed include time-of-flight mass spectrometry, energy analysis, collection and analysis of sputtered material, and scanning force microscopy. Characteristics of the sputtering process probed include the sputtering yield, radial and axial velocity distributions, angular distributions, and surface track morphology. Besides reviewing and correlating experimental results, we also emphasize the common quasi-thermal origin of pressure-pulse/hydrodynamic and evaporative spike sputtering models.     

Comprehensive analysis of binary events in heavy ion reactions observed with dielectric track detectors

The dielectric track detectors are very efficient in registering the main fragments of a heavy ion reaction in the presence of lightly ionizing products and γ-radiations because of their threshold nature of registration and wide-angle acceptance. The binary events, revealed after chemical etching of these detectors, appear as the events having two correlated prongs in the body of the detector. The measurements of the geometrical parameters of these prongs provide the necessary data for subsequent kinematical analysis. We have made a thorough analysis of the two-pronged events in order to understand the physical mechanism of their production, using the track data from the reactions,     

The pore opening process of etching polymer films irradiated by single and multiple heavy ions. The etching process in the range of the track core radius (10 nm)

The technique of electrochemical etching of irradiated polymer films is an useful method to investigate structures of the track cores. In the case of the investigation of multiple track foils, the mean effective radius corresponds to the average of all synchron etching pores. On the other hand, the etching cones of all tracks do not break through to conducting micro channels coincidentally. The statistical character of this pore opening (break through) process is still unexplained, although several effects concerning this topic have been observed in the past. Another computer program simulates by way of the Monte Carlo Method the etching process of an ensemble of tracks within a thin polymer film. The conductivity of the multiple track etching foil can be described by the convolution between the conductivity of a single pore and the time dependent breakthrough rate. By way of the Laplace Transforms the measurements of the multiple and single track etching polymer films can be deconvoluted and yield the statistical nature of the pore opening process.     

Study of spatial structure and energy spectrum of ion beams by means of LR 115A and PM-355 nuclear track detectors

The paper reports on measurements of pulsed plasma-ion streams, as performed with the selected solid-state nuclear track detectors (SSNTD). The ion-beams were produced by an experimental device (RPI-IBIS) equipped with coaxial electrodes (each made of molybdenum rods) and a fast-acting gas valve. The device was operated at 30 kV/44 kJ, with puffing of pure hydrogen or deuterium. The spatial structure of the ion beams was studied with pinhole cameras equipped with replaceable detectors, and ion mass- and energy-spectra were measured with a Thomson spectrometer. To analyse low-energy ions (below the energy thresholds of LR 115A and PM-355 SSNTD) an additional accelerating system was applied. It was observed that ions of energy are emitted in bunches, and the ion flux amounts to at a distance of 30 cm from the electrodes outlet. Energy spectra of protons and deuterons ranged from about 30 keV to about 400 keV. The ion distributions, as recorded by means of the PM-355 and LR 115A detectors, are similar.     

Damage processes in Fe 3 O 4 magnetic insulator irradiated by swift heavy ions. Experimental results and modelisation

The behavior of the magnetic properties of magnetite Fe₃O₄ irradiated by swift heavy ions is investigated by magnetization measurements. Although there is no induced structural phase transformation, both coercive field and saturation magnetization are sensitive to ion irradiation and exhibit different behaviors depending on the ion fluence range. In the low fluence regime, the coercive field increases, which is evidence for a strong pinning of magnetic domain boundaries by the induced defects. The magnetization shows a decrease in the saturation value and tends to reorient perpendicularly to the ion track axis. At high fluence, the initial magnetic properties of the sample are nearly restored. The changes in the magnitude and the direction of magnetization are interpreted by magnetostrictive effects related to the stress induced by irradiation. A phenomenological model is applied to reproduce the fluence evolution of the saturation magnetization, assuming relaxation of the stress induced around the core of defects of the tracks by overlapping effects at high fluence. The results are compared to those obtained in the case of yttrium iron garnet Y₃Fe₅O₁₂. Received 18 April 2001 and Received in final form 24 July 2001     

Damage morphology of Kr ion tracks in apatite: dependence on dE/dX

With the aim of characterizing damage along nuclear tracks in apatite, Durango fluoroapatite monocrystals were irradiated under a high fluence ⁸⁶Kr ion beam at the G.A.N.I.L. (Grand Accélérateur National d'Ions Lourds, Caen, France). The resulting irradiation damage was studied by associating CRBS spectrometry and chemical etching. By applying Poisson's law to the backscattering results, the nuclear track average effective radius R_e was calculated for different steps along the ion path. On the other hand, the chemical etching experiments allowed us to deduce three different damaging morphologies in correspondence to the R_e values. For the first time in apatite, it has been shown that a defect fragmentation produced along the ion paths may be detected by chemical etching. These results were also applied to fission tracks in order to quantify the damage rate and to describe the damage morphology evolution along fission fragment paths.     

Investigation of point defects in silicon and germanium by non-irradiation techniques

We have derived a simple empirical formula for sputtering yields of monatomic metals and semiconductors, taking the threshold effect for knock-on of atoms into account in the Sigmund theory. It is found that this semi-empirical formula fits to the energy dependence of the sputtering yields over a wide range of ion-target combinations. The best fit values of the parameters for the formula are given as a function of the ratio of the mass of target atoms and the mass of incident ions.     

Solvation structure of magnesium,zinc, and alkaline earth metal ions in N,N‐dimethylformamide,N,N‐dimethylacetamide,and their mixtures studied by means of Raman spectroscopy and DFT calculations—Ionic size and electronic effects on steric congestion

The solvation structure of magnesium, zinc(II), and alkaline earth metal ions in N,N‐dimethylformamide (DMF) and N,N‐dimethylacetamide (DMA), and their mixtures has been studied by means of Raman spectroscopy and DFT calculations. The solvation number is revealed to be 6, 7, 8, and 8 for Mg²⁺, Ca²⁺, Sr²⁺, and Ba²⁺, respectively, in both DMF and DMA. The δ (O C N) vibration of DMF shifts to a higher wavenumber upon binding to the metal ions and the shift Δν(= ν_bound − ν_free) becomes larger, when the ionic radius of the metal ion becomes smaller. The ν (N CH₃) vibration of DMA also shifts to a higher wavenumber upon binding to the metal ions. However, the shift Δν saturates for small ions, as well as the transition‐metal (II) ions, implying that steric congestion among solvent molecules takes place in the coordination sphere. It is also indicated that, despite the magnesium ion having practically the same ionic radius as the zinc(II) ion of six‐coordination, their solvation numbers in DMA are significantly different. DFT calculations for these metalsolvate clusters of varying solvation numbers revealed that not only solvent–solvent interaction through space but also the bonding nature of the metal ion plays an essential role in the steric congestion. The individual solvation number and the Raman shift Δν in DMF–DMA mixtures indicate that steric congestion is significant for the magnesium ion, but not appreciable for calcium, strontium, and barium ions, despite the solvation number of these metal ions being large. Copyright © 2006 John Wiley & Sons, Ltd.