Ion Track Formation Research Articles

Development of highly sensitive electrochemical immunosensor using PPy-MoS2-based nanocomposites modified with 90MeV C6+ ion beams.

Theevaluation of electrochemical sensing activity of hydrothermally derived PPy-MoS2-based nanocomposites subjected to 90MeV C6+ ion beam with fluence ranging, 1.0 × 1010-1.0 × 1013 ions/cm2, is reported. Cross-linking, chain scissioning, and ion track formation could occur in the irradiated systems, as revealed from Fourier transform infrared (FTIR) spectroscopy and field emission scanning electron microscopy (FE-SEM)studies. Electrochemical studies, viz., cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were performed in 0.1M phosphate buffer solution (PBS) containing 5mM K3[Fe(CN)6] as redox probe. High redox activity, lower charge transfer resistance (Rct = 490 Ω) and larger electroactive area (A = 0.4485 cm2) were obtained in case of the composite system irradiated with a fluence of 3.5 × 1011 ions/cm2. Immunosensor fabrication was executed via immobilization of mouse IgG over the pristine and post-irradiated electrodes. Afterwards, differential pulse voltammetry (DPV) was performed within thepotential window - 0.2 to + 0.6V (vs. Ag/AgCl) for the detection of specific analyte. Noticeably, the electrode system irradiated with a fluence of 3.5 × 1011 ions/cm2 ischaracterized by a lower limit of detection (LOD) of 0.203nM and a higher sensitivity value of 10.0 µAmLng-1cm-2. The energetic particle irradiation at a modest fluence can offer beneficial effects to thePPy-MoS2-based nanohybrid system providing immense scope as advanced electrochemical biosensor.

Latent ion tracks were finally observed in diamond

Injecting high-energy heavy ions in the electronic stopping regime into solids can create cylindrical damage zones called latent ion tracks. Although these tracks form in many materials, none have ever been observed in diamond, even when irradiated with high-energy GeV uranium ions. Here we report the first observation of ion track formation in diamond irradiated with 2–9 MeV C60 fullerene ions. Depending on the ion energy, the mean track length (diameter) changed from 17 (3.2) nm to 52 (7.1) nm. High resolution scanning transmission electron microscopy (HR-STEM) indicated the amorphization in the tracks, in which π-bonding signal from graphite was detected by the electron energy loss spectroscopy (EELS). Since the melting transition is not induced in diamond at atmospheric pressure, conventional inelastic thermal spike calculations cannot be applied. Two-temperature molecular dynamics simulations succeeded in the reproduction of both the track formation under MeV C60 irradiations and the no-track formation under GeV monoatomic ion irradiations.

Nanoscale core-shell structure and recrystallization of swift heavy ion tracks in SrTiO3.

It is widely accepted that the interaction of swift heavy ions with many complex oxides is predominantly governed by the electronic energy loss that gives rise to nanoscale amorphous ion tracks along the penetration direction. The question of how electronic excitation and electron-phonon coupling affect the atomic system through defect production, recrystallization, and strain effects has not yet been fully clarified. To advance the knowledge of the atomic structure of ion tracks, we irradiated single crystalline SrTiO3 with 629 MeV Xe ions and performed comprehensive electron microscopy investigations complemented by molecular dynamics simulations. This study shows discontinuous ion-track formation along the ion penetration path, comprising an amorphous core and a surrounding few monolayer thick shell of strained/defective crystalline SrTiO3. Using machine-learning-aided analysis of atomic-scale images, we demonstrate the presence of 4-8% strain in the disordered region interfacing with the amorphous core in the initially formed ion tracks. Under constant exposure of the electron beam during imaging, the amorphous part of the ion tracks readily recrystallizes radially inwards from the crystalline-amorphous interface under the constant electron-beam irradiation during the imaging. Cation strain in the amorphous region is observed to be significantly recovered, while the oxygen sublattice remains strained even under the electron irradiation due to the present oxygen vacancies. The molecular dynamics simulations support this observation and suggest that local transient heating and annealing facilitate recrystallization process of the amorphous phase and drive Sr and Ti sublattices to rearrange. In contrast, the annealing of O atoms is difficult, thus leaving a remnant of oxygen vacancies and strain even after recrystallization. This work provides insights for creating and transforming novel interfaces and nanostructures for future functional applications.

Fine structure of the tracks of several-tens-MeV Au ions in YBa2Cu3O7-x studied by cross-sectional transmission electron microscopy

We studied the morphology of the tracks (irradiation damage) of 44, 66, and 84 MeV Au ions in YBa2Cu3O7-x (YBCO) thin films using cross-sectional transmission electron microscopy (TEM). The electronic energy loss (Se = 11.6, 16.7, and 20.1 keV/nm) ranged near the onset of ion-track formation previously determined by plan-view TEM and critical-temperature measurements (about 13 keV/nm). The morphology changed from 1D arrays of large spheres of about 5 to 10 nm diameter in 44-MeV irradiation to their elongated variant (spheroid) that were statistically pierced by thin-lines of about 1 to 2 nm and 3 to 5 nm diameter in 66 and 84 MeV, respectively. In the same series of Au-irradiated YBCO films, we observed a sudden increase in critical current density at self-field and 77 K between 44- and 55-MeV irradiation, in agreement with the appearance of the thin-line damage in TEM (between 44- and 66-MeV).

The effect of aluminium concentration on the resistance of Si3N4 to ion track formation

The role of Al impurities on the structural response of polycrystalline silicon nitride to swift Xe and Bi ions at single ion track and overlapped ion track fluences is investigated. Si3N4 with Al impurity concentrations of 3 at.%, 1 at.% and 0.1. at.% were examined by means of high resolution scanning transmission electron microscopy. The threshold electronic energy loss (Set) required to form amorphous tracks was found to decrease with increasing Al fraction from above 33 keV/nm (0.1 at.% Al) to below 22 keV/nm for specimens containing about 3 at.% Al. All specimens were partially amorphized at overlapping ion fluence and the amorphous fraction monotonically increased with increasing Al content at the same ion fluence.

Suspended nanoporous graphene produced by swift heavy ion bombardment

In the present work, Raman spectroscopy measurements and molecular dynamics simulations were used to investigate damage production in suspended single-layer graphene when irradiated by 23 MeV I, 3 MeV Cu and 18 MeV Cu beams. Despite the high energies of the used swift heavy ion beams, we found no evidence of ion track formation, i.e. all damage imparted to graphene was due to elastic collisions between ions and carbon atoms. Comparing experimental results with simulations, we conclude that a significant amount of energy (at least 40 % in the case of 23 MeV I irradiation) is dissipated away from graphene following the ion impact, and is a likely reason for the absence of ion tracks.

Threshold for ionization-induced defect annealing in silicon carbide

Ion track formation in SiC has never been observed, but this material is well-known for easily achieving ionization-induced defect annealing. Therefore, the aim of this work is to study the threshold for ionization-induced defect annealing in silicon carbide using Rutherford backscattering spectrometry in channeling mode. It was established that 3 MeV O beam can activate the ionization-induced defect annealing in SiC, but 12 MeV O cannot, despite the same electronic stopping values. We attribute this finding to the velocity effect and propose systematic investigations of ionization-induced defect annealing with respect to the velocity of the ion beams used.

Ion track formation and porosity in InSb induced by swift heavy ion irradiation

Ion track formation, irradiation-induced damage (amorphization), and the formation of porosity in InSb after 185 MeV 197Au swift heavy ion irradiation are studied as a function of ion fluence and irradiation angle. Rutherford backscattering spectrometry in channeling geometry reveals an ion track radius of about 16 nm for irradiation normal to the surface and 21 nm for off-normal irradiation at 30° and 60°. Cross-sectional scanning electron microscopy shows significant porosity that increases when irradiation was performed off-normal to the surface. Off-normal irradiation shows a preferential orientation of the pores at about 45° relative to the surface normal. Moreover, when subjected to identical conditions, InSb samples demonstrate notably higher swelling compared to GaSb bulk samples.

Ion Track Formation and Nanopore Etching in Polyimide: Possibilities in the MeV Ion Energy Regime

AbstractPolyimide films of thickness 7.5 µm are irradiated by a wide range of ions (1H to 197Au) with energies between 1.05 and 48 MeV. Irradiated samples are then chemically etched in sodium hypochlorite solution to investigate nanopore formation due to ion track etching. A threshold in terms of electronic stopping power, Set, needs to be surpassed to preferentially etch the ion tracks. Close to Set, intermittent tracks are formed where only part of the track is etchable. The fraction of these etchable parts increases as we move away from Set, toward higher stopping powers, eventually yielding continuous etchable tracks. Both intermittent and continuous track formation thresholds are observed to be velocity‐dependent, yielding a decrease of the thresholds in the present work compared to previously reported thresholds for swift heavy ions. This finding leads the authors to suggest that electrostatic ion accelerators with terminal voltages of several MV are applicable for the production of ion track membranes up to ≈10–20 µm in thickness. Suitable ions for nanopores in 7.5 µm polyimide films include 42 MeV 59Co and 48 MeV 197Au. The growth mechanism for the pores during etching is discussed, relating it to the properties of the original ion track.

In situ luminescence from MgOAl2O3 irradiated by swift heavy Xeq+ ions

Ion irradiation can result in luminescence emission from optical window material aluminum magnesium spinel (MgOAl2O3). In the present work, single crystals of MgOAl2O3 are irradiated with swift heavy ions. During irradiation, the emission spectra, in the range of 200–800 nm, are obtained from MgOAl2O3 irradiated by 93–609 MeV Xeq+ ions. The emission bands originated from radiative recombination of excitons and the spectral lines derived from impurity ions are observed. These emission bands, as a function of incident ion energy and irradiation dose, are presented. The results indicate that the increase of ion energy can effectively increase the spectral intensity, and due to crystal damage caused by ion irradiation, the spectral intensity decreases with increasing irradiation dose. Similar to nanohillock and ion track formation, luminescence emission occurs above a critical electronic energy loss of about 7.2 keV/nm. In-situ measurement of the luminescence emission is of great significance to study the irradiation modification and can help to understand the process of crystal damage caused by ion irradiation.

Mechanism of ion track formation in silicon by much lower energy deposition than the formation threshold

Mechanism of the ion track formation in crystalline silicon (c-Si) is discussed, particularly under 1–9 MeV C60 ion irradiation. In this energy region, the track formation was not expected because the energy E was much lower than the threshold of E th = 17 MeV determined by extrapolation from higher energy data in the past literature. The track formation is different between irradiations of C60 ions and of monoatomic ions: The tracks were observed under 3 MeV C60 ion irradiation but not under 200 MeV Xe ions, while both the irradiations have the same electronic stopping (S e) of 14 keV nm−1 but much higher nuclear stopping (S n) for the former ions. The involvement of S n is suggested for the C60 ions. While the inelastic thermal spike (i-TS) calculations predict that the high energy monoatomic ion irradiation forms the tracks, the tracks have never been experimentally detected, suggesting quick annihilation of the tracks by highly enhanced recrystallization in c-Si. Exceptions are C60 ions of 1–9 MeV, where the track radii are well reproduced by the i-TS theory with assuming the melting transition. Collisional damage induced by the high S n from C60 ions obstructs the recrystallization in c-Si. Then the tracks formed by the melting transition survive against the recrystallization. This is a new type of the synergy effect between S e and S n, different from the already-known mechanisms, i.e., the pre-damage effect and the unified thermal spike. While c-Si was believed as a radiation-hard material in the S e regime with high S e threshold, this study suggests that c-Si has a low S e threshold but with efficient recrystallization.

Illustrating the atomic structure and formation mechanism of ion tracks in polyethylene terephthalate with molecular dynamics simulations

This work reports molecular dynamics (MD) simulations of the formation of detailed ion track structures at the atomic scale in polymers. To simulate the initial chemical reactions and the subsequent thermal movement of polymer molecules, an adapted thermal spike model was implemented using a charge-implicit reactive force field potential. The MD simulation reproduces the physical–chemical process of ion track formation observed in the experiment, e.g., the bond breakage and creation, gas production and release, carbonization effect, and the relative radial density distributions, which are consistent with small angle X-ray scattering results of ion tracks in polyethylene terephthalate generated with 15.9 keV nm−1 Au and 10.9 keV nm−1 Xe ions, respectively. Based on the MD simulation, the ion tracks in polymers show a heavily-damaged core region with an inhomogeneous nanoporous structure, and a surrounding transition region with the mass density increasing gradually back to the same value as the pristine sample.

High-Energy Heavy Ion Tracks in Nanocrystalline Silicon Nitride

At present, silicon nitride is the only nitride ceramic in which latent ion tracks resulting from swift heavy ion irradiation have been observed. Data related to the effects of SHIs on the nanocrystalline form of Si3N4 are sparse. The size of grains is known to play a role in the formation of latent ion tracks and other defects that result from SHI irradiation. In this investigation, the effects of irradiation with high-energy heavy ions on nanocrystalline silicon nitride is studied, using transmission electron microscopy techniques. The results suggest that threshold electronic stopping power, Set, lies within the range 12.3 ± 0.8 keV/nm to 15.2 ± 1.0 keV/nm, based on measurements of track radii. We compared the results to findings for polycrystalline Si3N4 irradiated under similar conditions. Our findings suggest that the radiation stability of silicon nitride is independent of grain size.

Modeling fission spikes in nuclear fuel using a multigroup model of electronic energy transport

In fission based nuclear reactors the fuel is subject to an intense neutron environment that drives the fission chain reaction. Due to this process fission fragments are created with energies reaching 1 MeV/amu that lose energy primarily through inelastic interactions with the electronic structure producing electronic excitations. Subsequently, these excitations thermalize through electron-phonon interactions resulting in the formation of a high temperature thermal spike and associated pressure spike. This process promotes atomic mobility that is expected to evolve lattice defects, including the annealing of latent ion tracks. In this work, a multigroup model for electron energy transport is developed and applied to molecular dynamics simulations in the LAMMPS code to examine fission energy deposition and fission effects in nuclear fuel. This technique utilizes MCNP Monte Carlo electron transport calculations to determine the initial injection of fission energy. To provide a more predictive approach than semi-empirical two-temperature models, the electron-phonon interactions are defined to include multiphonon energy transfer as a function of atomic and electron temperature, and are evaluated from electronic structure calculations using the VASP density functional theory code and PHONON lattice dynamics code. Application of this model to fission energy deposition in uranium dioxide predicts ion track formation and fission enhanced atomic mobility behavior within reasonable agreement of experimental trends. Furthermore, simulations of fission fragment interactions with latent ion tracks demonstrate an annealing effect due to this enhanced mobility.

Surface nanostructures on Nb-doped SrTiO3 irradiated with swift heavy ions at grazing incidence

A single crystal of SrTiO3 doped with 0.5 wt% niobium (Nb-STO) was irradiated with 200 MeV Au32+ ions at grazing incidence to characterize the irradiation-induced hillock chains. Exactly the same hillock chains are observed by using atomic force microscopy (AFM) and scanning electron microscopy (SEM) to study the relation between irradiation-induced change of surface topography and corresponding material property changes. As expected, multiple hillocks as high as 5–6 nm are imaged by AFM observation in tapping mode. It is also found that the regions in between the adjacent hillocks are not depressed, and in many cases they are slightly elevated. Line-like contrasts along the ion paths are found in both AFM phase images and SEM images, indicating the formation of continuous ion tracks in addition to multiple hillocks. Validity of preexisting models for explaining the hillock chain formation is discussed based on the present results. In order to obtain new insights related to the ion track formation, cross-sectional transmission electron microscopy (TEM) observation was performed. The ion tracks in the near-surface region are found to be relatively large, whereas buried ion tracks in the deeper region are relatively small. The results suggest that recrystallization plays an important role in the formation of small ion tracks in the deep region, whereas formation of large ion tracks in the near-surface region is likely due to the absence of recrystallization. TEM images also show shape deformation of ion tracks in the near-surface region, suggesting that material transport towards the surface is the reason for the absence of recrystallization.

Depth-resolved thermal conductivity and damage in swift heavy ion irradiated metal oxides

We investigated thermal transport in swift heavy ion (SHI) irradiated insulating single crystalline oxide materials: yttrium aluminum garnet- Y3Al5O12 (YAG), sapphire (Al2O3), zinc oxide (ZnO) and magnesium oxide (MgO) irradiated by 167 MeV Xe ions at 1012 – 1014 ions/cm2 fluences. Depth profiling of the thermal transport on nano- and micro- meter scales was assessed by time-domain thermoreflectance (TDTR) and modulated thermoreflectance (MTR) methods, respectively. This combination allowed us to isolate the conductivities of different sub-surface damage-regions characterized by their distinct microstructure evolution regimes. Thermal conductivity degradation in SHI irradiated YAG and Al2O3 is attributed to formation of ion tracks and subsequent amorphization, while in ZnO and MgO it is mostly due to point defects. Additionally, notably lower conductivity when probed by very low penetrating thermal waves is consistent with surface hillock formation. An analytical model based on Klemens-Callaway method for thermal conductivity coupled with a simplified microstructure evolution capturing saturation in defect concentration was used to obtain depth dependent damage across the ion impacted region. The studies showed that YAG has the highest damage profile resulting in the less dependence of thermal conductivity with the depth, while MgO on the contrary has the strongest dependence. The presented work sheds new light on how SHI induced defects affect thermal transport degradation and recovery of oxide ceramics as promising candidates for next generation nuclear reactor applications.

Incident Angle Dependent Formation of Ion Tracks in Quartz Crystal with C60+ Ions: Big Ions in Small Channels

Quartz (SiO2) crystals possess intrinsic columnar pores perpendicular to (0001) surfaces, consisting of three- and six-membered ring (3MR and 6MR) structures of Si and O atoms. The diameters of the larger pores, i.e., 6 MRs, are ~0.49 nm, while the diameters of fullerene (C60) ions are 0.7 nm, i.e., larger than either type of the pores. Transmission electron microscopy observation evidenced approximately two times longer ion tracks in the channeling condition, i.e., 0° incidence to (0001) surface, than an off-channeling condition, i.e., 7° incidence in this case, under 6 MeV C60 ion injection. The track length at the 0° incidence decreases more steeply than that at the 7° incidence with decreasing the energy from 6 MeV to 1 MeV. Finally, the track lengths at the 0° and 7° incidences become comparable, i.e., the channeling-like effect disappears at 1 MeV irradiation. This study experimentally indicates that the channeling-like effect of C60 ions is induced in quartz crystals, while the sizes of the channels are smaller than the C60 ions.

Swift heavy ion induced phase transformations in partially stabilized ZrO2

The paper reports on the effect of irradiation by swift heavy Xe ions on partially stabilized zirconia ceramics. XRD analysis identified two tetragonal phases with different degrees of tetragonality (transformable t phase and non-transformable metastable t” phase). TEM analysis of the irradiated samples showed that the efficiency of high-energy ion track formation decreases when the fluence and, hence, the fraction of t” phase increase. Changes in nanohardness, elastic modulus, and microhardness of partially stabilized ZrO2 ceramics before and after irradiation were investigated by nanoindentation and microindentation techniques. Mechanisms of ceramic layer hardening associated with phase rearrangement, compressive stress accumulation, and transformation and ferroelastic hardening are discussed.

Energy Retention in Thin Graphite Targets after Energetic Ion Impact.

High energy ion irradiation is an important tool for nanoscale modification of materials. In the case of thin targets and 2D materials, which these energetic ions can pierce through, nanoscale modifications such as production of nanopores can open up pathways for new applications. However, materials modifications can be hindered because of subsequent energy release via electron emission. In this work, we follow energy dissipation after the impact of an energetic ion in thin graphite target using Geant4 code. Presented results show that significant amount of energy can be released from the target. Especially for thin targets and highest ion energies, almost 40% of deposited energy has been released. Therefore, retention of deposited energy can be significantly altered and this can profoundly affect ion track formation in thin targets. This finding could also have broader implications for radiation hardness of other nanomaterials such as nanowires and nanoparticles.

Stoichiometry dependent changes in the optical properties and nanoscale track formation of PECVD grown a-SiNx:H thin films upon 100 MeV Au8+ ion irradiation

a-SiNx:H thin films of different stoichiometry grown by PECVD were subjected to irradiation by 100 MeV Au8+ ions with various fluences to understand the effect of stoichiometry on properties of thin films upon irradiation. Ellipsometry and UV–Vis study suggest the variation in the refractive index of thin films with fluence. The evolution of Hydrogen due to irradiation is quantified with the help of ERDA. RBS was probed to study the change in thin films' composition upon irradiation, which further helps understand the change in thin films' optical properties. Quenching of photoluminescence in the films with all stoichiometries was also observed due to ion irradiation. X-TEM images show the formation of discontinuous ion tracks of radius 2.5 nm in the film closer to silicon nitride stoichiometry. However, Si rich film does not show the clear formation of tracks. Results are explained in the framework of the Thermal spike mechanism of ion-solid interaction.