Four decades of nuclear tracks research in India

The science of solid state nuclear track detectors (SSNTDs)—“Trackology”—developed by R.L. Fleischer, P.B. Price and R.M. Walker in the early 1960s of the last century is an interesting and potentially useful concept with something to offer to almost all branches of science and technology. In fact nuclear tracks find applications wherever solid state damage occurs. Apart from the direct applications of far reaching consequences in nuclear physics, other areas as diverse as bio-medical sciences, cosmic rays and space physics, environmental research, geological sciences, material science, microanalysis, mine safety, nuclear technology, uranium prospecting, etc. have been greatly influenced by SSNTDs.

In this presentation, we attempt to provide an overview of the growth of nuclear tracks research in India over the last four decades and the contributions of various groups from Universities, Institutes, Nuclear Track Society of India and the Department of Atomic Energy in nurturing nuclear track research in the country. Finally, a summary of the significant contributions made by Indian scientists is also presented in this paper along with the overall impact it has made at the national and international level in many areas of basic and applied sciences such as cosmic rays and space physics, fusion–fission and particle evaporation, heavy ion ranges and energy-loss measurements, country-wide indoor radon–thoron survey, geochronology, environmental sciences, track-etch membranes and ion tracks technology, material science, physics and chemistry of fission, etc.     

The effect of UV exposure on the track and bulk etching rates in different CR-39 plastics

It is observed that for both UK and Japanese CR-39 detectors the mean diameters of fission fragment and alpha tracks from a Cf-252 source become larger as a result of UV exposure; but in the case of ‘UV exposure last’ (i.e. Cf + UV) the diameters are larger than in the case of ‘UV exposure first’ (i.e. UV + Cf). The bulk and track etching rates undergo an increase with UV exposure for the two kids of CR-39.     

AFM observations of latent fission tracks on surfaces: amorphous SiO2 and quartz

Preliminary results of a systematic AFM experimental investigation of the surface ‘track’ effects produced by the passage of fission fragments from a californium (²⁵²Cf) source into amorphous SiO₂ and quartz are described. Fission fragments from the source were collimated using a 10 μm thick aluminum foil and comprised fragments with the usual binary distribution of energies—light and heavy—79.4 and 103.8 MeV. Irradiations and AFM measurements were carried out in air at normal room temperature and pressure. Remarkably high sputtering yields/fragment were discovered, and in the case of crystalline quartz the ejecta was found to be arranged in an ordered manner. A brief discussion is given of a part likely to be played by electronic energy loss induced Coulomb explosion of target atoms for each point of fragment entry.     

Cosmic history of the Bragin pallasite: evidence from the fission-track analysis

Chronology is rather a weak point in the investigation of pallasites, the stony-iron meteorites. No chronological data are known for the Bragin pallasite. Our attempt to reconstruct its cosmic history was based on the interpretation of fission-track analysis data. To apply this method only uranium-rich phosphates can be used. Extremely rare grains of stanfieldite were extracted from the silicate sawing residue and from the pallasite sample directly.

The researches pursued by us made it possible to find two populations of fossil tracks in stanfieldite grains. The tracks of these populations strongly differed both in size, shape and character of distribution. The first population, consisting of short (L2–6 μm instead of L8–12 μm for induced fission tracks), round-shaped tracks irregularly distributed, as we suppose, suffered an intense heating process, which caused a significant amount of partial annealing. The second population, consisting of longer (L8–12 μm), rhombic-shaped tracks homogeneously distributed, occurred after this thermal event. Only the second population track density was used for the fission-track age calculation.

After correction of the fossil track density, consisting of the second population tracks, for other possible track sources, the revealed tracks were unequivocally identified as those due to the spontaneous fission of ²⁴⁴Pu and ²³⁸U. The largest part of them was attributed to the spontaneous fission of ²⁴⁴Pu; ρ_Pu/ρ_U≈3. The model fission-track age of the studied pallasite turned out to be 4.20 Gyr. This value fix the time of the last shock/thermal event in the cosmic history of the Bragin pallasite, which had caused the partial annealing of tracks presented to that time and “fission-track clock” reset.     

Radiation damage to DNA: the importance of track structure

A wide variety of biological effects are induced by ionizing radiation, from cell death to mutations and carcinogenesis. The biological effectiveness is found to vary not only with the absorbed dose but also with the type of radiation and its energy, i.e., with the nature of radiation tracks. An overview is presented of some of the biological experiments using different qualities of radiation, which when compared with Monte Carlo track structure studies, have highlighted the importance of the localized spatial properties of stochastic energy deposition on the nanometer scale at or near DNA. The track structure leads to clustering of damage which may include DNA breaks, base damage etc., the complexity of the cluster and therefore its biological repairability varying with radiation type.

The ability of individual tracks to produce clustered damage, and the subsequent biological response are important in the assessment of the risk associated with low-level human exposure. Recent experiments have also shown that biological response to radiation is not always restricted to the ‘hit’ cell but can sometimes be induced in ‘un-hit’ cells near by.     

Nuclear track radiography of “Hot” aerosol particles

Nuclear track radiography was applied to identify aerosol “hot” particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the -activity of “hot” particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and (γ,f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of “hot” particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by ²³⁵U, ²³⁹Pu and ²⁴¹Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5×10⁻⁶ Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical image of the SSNTD surface obtained through a video camera and the determination of size and activity of “hot” particles.     

Hollow particle tracks in AgCI-detectors

In selected Cd-doped monocristalline silverchloride detectors we observe developed tracks from particles at LET values > 300 keV/μm AgCl and charge state values > 9, without a visible central region: the “hollow track”. The microdensitometric lateral profile shows a density decrease near the track axis, up to a radial extension of some microns from highly charged particles as Fe or U-ions of several MeV/u; the tracks of fast U- or Fe-projectiles, moreover, represent an entanglement of delta-electron tracks only. A recent reanalysis of this “hollow track”-effect is suggested to be caused by recombination effects and structural distortions. They occure in areas of high delta-electron density; together with the characteristic process of track formation in crystalline AgCl/Cd they enable us to vizualise and to measure the radial range of distortion and to evaluate the threshold of the energy density above which the destruction occurs.     

Thermal spike analysis of low energy ion tracks

The theoretical track diameter of low energy ions in organic materials is usually estimated through the model of dose deposition by delta rays, with results remarkably lower than the experimental values obtained via a replica method and electron microscopy. The track detector used here is Makrofol-E and the ions studied have specific energies between 1.4 and 100 keV/n. To evaluate the problem from another point of view, thermal effects for track formation, a modified version of the “liquid drop model” for insulators was applied. The electronic as well as nuclear energy deposition by an individual ion are considered and the thermal spike evolution is studied. The model allows for the formation of ion tracks in a range of energies previously considered as “forbidden”. There still exists a discrepancy between the experimental data and the track diameters predicted by the model, and although this difference is smaller than the obtained with previous calculations, it suggests the necessity of further adjustments.     

Conductivity of aged non-overlapping and overlapping tracks in ion irradiated polyimide

Non-overlapping as well as overlapping tracks of energetic ions have been introduced into polyimide foils. After aging their conductivity was measured. This — to our knowledge — first systematic study shows that conductivity does not only result from multiple track overlapping, but can be found already in single ion tracks. This conductivity is shown to be primarily a consequence of electronic energy transfer. The conductivity of single ion tracks is higher than that of typical insulators, but still orders of magnitude lower than that of typical semiconductors. The conductivity is independent of the applied electric field strength until at excessive voltages the electric current increases nonlinearly up to complete breakthrough. The total conductivity of an irradiated polyimide foil increases proportionally with ion fluence for large ion track spacings, and approaches saturation when the electronically active track regimes begin to overlap. Above some thousand times track overlapping however, new chemical and structural changes in the irradiated material lead to another strong increase in conductivity.     

On methodical problems in estimating geological temperature and time from measurements of fission tracks in apatite

The results of apatite fission-track modelling are only as accurate as the method, and depend on the assumption that the processes involved in the annealing of fossil tracks over geological times are the same as those responsible for the annealing of induced fission tracks in laboratory experiments. This has hitherto been assumed rather than demonstrated. The present critical discussion identifies a number of methodical problems from an examination of the available data on age standards, borehole samples and samples studied in the framework of geological investigations. These problems are related to low- (<60°C) and high-temperature (>60°C) annealing on a geological timescale and to the procedures used for calculating temperature–time paths from the fission-track data. It is concluded that it is not established that the relationship between track length and track density and the appearance of unetchable gaps, observed in laboratory annealing experiments on induced tracks, can be extrapolated to the annealing of fossil tracks on a geological timescale. This in turn casts doubt on the central principle of equivalent time.

That such uncertainties still exist is in no small part due to an insufficient understanding of the formation, structure and properties of fission tracks at the atomic scale and to a lack of attention to the details of track revelation. The methodical implications of discrepancies between fission track results and the independent geological evidence are rarely considered. This presents a strong case for the re-involvement of track physicists in fundamental fission track research.     

Alternative procedure for LR 115 chemical etching and alpha tracks counting

An improved procedure for etching and analysis of alpha tracks induced in LR-115 detectors is proposed with the advantages of simplicity and its relatively low cost. A new type of detector holder was designed to etch and rinse efficiently up to 100 detectors. We develop a simple and reliable methodology with a semiautomatic track count using a Nikon digital camera coupled to a PC and employing software “SCION” freely available on the Internet. Track images are binarized prior the application of software “SCION” so that original track shapes are not distorted, space resolution is improved and track counting has low dependence on focus and illumination level. High discrimination for tracks is achieved when marks and rips perturb the detector surface. An image generator of nuclear tracks is included to study the effect of track overlapping effect on counting.     

Surface fission tracks in diamond

Scanning Probe Microscope (SPM) images reveal important fingerprint features of latent tracks induced in diamond by fission fragments from a californium source. Collimated fission fragments with a binary distribution of the predominant energies of 79.4 and 103.8 MeV, are assumed. Cavities, reticular formations around these cavities, and black spots of graphite were found. A brief discussion on the possible track formation mechanism is given on the basis of the explosion spike theory; an attempt to determine latent track core and halo parameters is included.     

Nuclear tracks: present and future perspectives

Current research work related to the development of nuclear tracks comprising: (i) fundamental principles (nuclear track physics and chemistry, as well as development of track detectors and the relevant hard- and software), (ii) development of nuclear instruments and methods (etch track radiometers for ions, neutrons and cosmic rays, radon monitoring devices, radiography and fission track dating) is briefly outlined. The paper concentrates on a literature survey of applications of nuclear tracks in (iii) physical sciences (high-energy physics, nuclear physics and earth sciences), (iv) biomedical sciences (radiation protection, environment, cancer therapy), and (v) technological sciences (materials, nano-technology and nuclear technology).

Presently about 350 papers per year are being published in this field. Increased activity is noted in ion track technology (track-made membranes, modern nano-tech methodology including biological and biological-like samples, nano-electrode bio-electrochemistry, bio-magnetic assays and probes). New applications of nuclear tracks in fundamental (possibility of the detection of neutron quantum states in a gravitational field, nucleus–nucleus interactions, search for new chemical super-heavy elements) and applied science (precise measurements of the behaviour of radiation in human tissue in connection with of long term space missions and treatment of cancer) are surveyed, and possible research in the next decades is presented and examined in this review paper.     

Comparison of ‘blue’ and ‘infrared’ emission bands in thermoluminescence of alkali feldspars

Dating quaternary sediments by thermoluminescence (TL) or optically stimulated luminescence (OSL) calls for a detailed knowledge of the luminescence of feldspars. TL of the various alkali feldspars ((K, Na) Si₃AlO₈) display many common features, and some of these cause great difficulties for dating. After long storage following ionizing irradiation, the TL of most alkali feldspars is known to fade away by “anomalous fading”, which is incompatible with dating. This effect had been attributed to tunnel recombination. Following irradiation, a very intense tunnelling afterglow is observed at temperatures down to liquid nitrogen, in accordance with the observed rate of fading. This emission has a Gaussian spectrum entirely in the infrared (IR) with a maximum at 1.7 eV. It displays an important thermal quenching from 77 to 300 K. Its intensity is related with the ‘disorder’ of the crystal lattice. At higher temperatures, in TL proper, two emission bands can be separated. One is the well-studied complex visible emission, distributed over the spectral region from UV to orange, but mostly ‘blue’. The other is the ‘infrared’ band already observed at lower temperatures, which is attributed to Fe³⁺ ions. These two bands are clearly separated, with the spectral maxima, respectively, below and above 600 nm. They have also different kinetics, the glow peaks temperatures are different. But these two different bands are also coupled in many ways, they have parallel growth and fading. With ‘disordered’ feldspars, the ‘blue’ emission displays anomalous fading, which is stronger than that of the ‘infrared’. The infrared emission is more stable, which may be interesting for the purpose of dating.     

Radiation-induced processes and defects in alkali and alkaline-earth borate crystals

The paper presents the results of a study of the radiation-induced processes and defects in nonlinear optical crystals Li₂B₄O₇ (LTB), LiB₃O₅ (LBO), CsLiB₆O₁₀, KB₅O₈·4H₂O, β-BaB₂O₄. It was revealed that a pulsed electron beam irradiation at 290 K forms the radiation-induced pairs of the ‘vacancy—interstitial atom’ defects in the cation sublattice of these crystals. This gives rise to a creation of metastable electronic (interstitial atom) and hole (small-radius polaron near the cation vacancy) centers in high concentrations. Optical hole-transitions from the local level of the trapped hole centers to the valence band states are responsible for the transient optical absorptions (TOA) of borates in the visible and UV spectral ranges. A sublattice of the weakly bound mobile lithium cations in LTB and LBO favors a spatial separation of the radiation-induced pair defects ‘hole polaron near Li-vacancy—mobile interstitial Li⁰ atom’. Their decay rated by the electron–hole nonradiative tunnel recombination determines a peculiar feature of the TOA decay kinetics in LTB and LBO.     

On search and identification of tracks due to short-lived SHE nuclei in extraterrestrial crystals

The unique approach for search and unambiguous identification of short-lived (T_1/2=10³–10⁷ years) superheavy nuclei in cosmic-ray products of the recent nucleosynthesis in our Galaxy are discussed.It is based on: (a) the ability of non-conducting crystals to register and to store for many million years the tracks due to fast nuclei with atomic number Z20 (“fossil” tracks);(b) calibrations of the said crystals with accelerated heavy ions (20Z92) and on revealing the volume etchable track length (VETL) of the fast nuclei coming to rest inside crystals—both of fossil and “fresh” tracks—to determine the charge distribution of cosmic-ray nuclei tracks and(c) the so-called “four-zone” model of tracks in crystals (and also glasses) which provides not only the VETL track length dependence for 20Z92 nuclei but also demonstrates the regular annealing behavior of VETL of 20Z92 nuclei in a broad temperature interval.This approach was first applied in the early 1980s to investigate the “fossil” tracks due to 22Z92 cosmic-ray nuclei in olivine crystals from meteorites-pallasite Marjalahti and Eagle Station.The discovery of Th–U cosmic-ray nuclei tracks in 1980 was unambiguously confirmed by calibrations of the same crystals with ²³⁸U, ¹⁹⁷Au and ²⁰⁸Pb accelerated ions in the late 1980s. More than 1600 tracks due to cosmic-ray actinide nuclei were measured during the last two decades of the 20th century.Also, 11 anomalously long tracks (track length exceeds by a factor (1.6±0.1) the track length due to Th–U nuclei were measured. The detailed analysis shows that at least 5 of these tracks could not be attributed to the Th–U nuclei. It means that now we have a preliminary proof on the existence Z110 nuclei in cosmic-rays. The abundance is Z110/Th–U=(1–3)×10⁻³ in Z110 freshly formed cosmic-rays (time interval 10³–10⁷ years).The method proposed can provide the necessary and sufficient conditions for the discovery of Z110 nuclei in nature.     

Dosimetry of 40 and 70 MeV/n O beams

Using CR-39 plastic track detectors the range values of ¹⁶O ions at two different energies (initially in the beam line, 39.97 MeV/n and 69.98 MeV/n) were measured after escaping the beam pipe and found to be (3050 ± 40) μm and (8210 ± 90) μm, respectively. The longitudinal and projected angular spread of oxygen ions of an initial energy of 69.98 MeV/n in the region of the Bragg peak was derived from the measured geometrical parameters of tracks. Based on a calibration curve (etch rate ratio vs total linear energy transfer in CR-39) and the measured track length distribution at the range end of oxygen ions, the complete depth dose profile of a 67.7 MeV/n ¹⁶O beam in CR-39 (plateau, extended Bragg peak and residual ionization caused by projectile like fragments) was obtained.     

Measurement of nanosize etched pits in SiO2 optical fiber conduit using AFM

Fission fragment tracks from ²⁵²Cf have been observed in SiO₂ optical fiber, using an atomic force microscope (AFM), after a very short chemical etching in hydrofluoric acid solution at normal temperature. The nuclear track starting and evolution process is followed by the AFM direct measurements on the material surface and beyond a fine layer of the surface material. The images of the scanned cones were determined observing the two predominant energies from ²⁵²Cf fission fragments and the development of the tracks in the 150 μm diameter optical fiber conduit.     

Measurement of apex angle of the prism using total internal reflection

Total internal reflection technique is examined critically for the measurement of apex angle of the prism. Recognition of the critical boundary completely specifies the apex angle ‘A’ of the prism by keeping constant the ratio of refractive index of sample fluid (n₁=1.4) to that of glass (n₂=1.7). Recording of observations in the laboratory is dependent upon whether the apex angle ‘A’ of prism is greater than or less than or equal to critical angle ‘r_c’. The minimum value of error function ‘χ’ in the proximity of Abbe angle explain the choice of Abbe type instruments and shown invariant by relating positive ‘₊’ and the negative angle of emergence ‘₋’. Using ray-tracing technique, an expression for the length of the critical boundary ‘l’ is derived and is shown as a measure of the apex angle ‘A’ of the prism.

The choice of the realistic grazing condition leads us to two turning points for which error function ‘χ’ is minimal and yields appropriate option of the measurement of apex angle ‘A’ of the prism. It is further shown that the small error ‘ζ’ crept in the apex angle ‘A’ of the prism can lead to a significant error in the design of Pulfrich type instruments.

Experimental measurements are in-line with the predictions made.     

Differentiation between tracks and damages in SSNTD under the atomic force microscope

We have observed three-dimensional sponge-like structures as well as strips of connecting pits on the surface of the LR 115 detector after etching, which can be confused with the small tracks formed after short etching time. We have employed an atomic force microscope (AFM) to study these “damages” as well as genuine alpha tracks for short etching time. It was found that while the track and damage openings could be similar in size and shape, the depths for the damages were consistently smaller. Therefore, the depth of the pits will serve as a clear criterion to differentiate between tracks and other damages. The ability to discriminate between genuine tracks from other damages is most important for etching for short time intervals.