Examining the residual radiological footprint of a former colliery: An industrial nuclear archaeology investigation.

Nuclear industrial archaeology utilises radiation mapping and characterisation technologies to gain an insight into the radiological footprint of industrial heritage sites. Increased concentrations of naturally occurring radioactive materials at legacy mine sites are the result of elemental enrichment during coal mining and subsequent combustion. Public safety is of concern around these sites, and therefore, an increased understanding of their associated hazard is essential. Using coincident laser scanning and gamma detection technologies, this study sought to assess the radiological legacy of a coal mine located in Bristol, UK. From this, we can increase our understanding of the residual footprints associated with the local coal mining industry. Samples taken from inside the site were characterised using high resolution gamma spectrometry, wherein the radionuclide content and activities of samples were then quantified. An area of elevated low-level radioactivity was observed at and around buildings believed to belong to the colliery, while Th, U, and K are confirmed at the site from photopeak's of daughter radionuclides. Activities of the radionuclides K-40, U-238, and Th-232 were further quantified during subsequent laboratory analysis. Results highlight an enrichment of naturally occurring radionuclides when compared with global averages for unburned coal. Employing these techniques at further legacy sites would enable an increased understanding of the lasting traces of the coal mining industry, with a focus on NORM enrichment in residual fly ash.

Modelling 'Type B' ejecta formation reveals reactor Unit 1 conditions during the Fukushima Daiichi Nuclear Disaster.

For the first time, a model was developed to simulate the cooling of the Fukushima Daiichi Nuclear Power Plant reactor Unit 1-derived, 'Type B' radiocaesium bearing microparticles, distributed into the environment during the 2011 nuclear meltdown. By establishing an analogy between 'Type B' CsMP and volcanic pyroclasts, the presented model simulates the rapid cooling of an effervescent silicate melt fragment upon atmospheric release. The model successfully reproduced the bi-modal distribution of internal void diameters observed in 'Type B' CsMP, however, discrepancies resulted primarily due to the neglection of surface tension and internal void coalescence. The model was subsequently utilised to estimate the temperature within reactor Unit 1 in the instant preceding the hydrogen explosion-between 1900 and 1980 K. Such a model demonstrates the accuracy of the volcanic pyroclast-'Type B' CsMP analogue, and confirms radial variations in cooling rate as the cause of the vesicular texture of Unit 1 ejecta. The presented findings provide scope to further explore the comparison between volcanic pyroclasts and 'Type B' CsMP via experimentation, which will provide a deeper understanding of the specific conditions within reactor Unit 1 during the catastrophic meltdown at the Japanese coastal plant.

A highly scalable and autonomous spectroscopic radiation mapping system with resilient IoT detector units for dosimetry, safety and security.

Technologies utilizing radiological materials across power generation, defence, industry, research and medicine have increased the global inventory of highly active and hazardous materials. Consequently, an amplified threat exists of illicitly obtained materials being used as part of hostile acts. The potential for intentional releases occurs alongside risks from natural disasters or facility accidents. In any such event, it is crucial to rapidly assess the release composition and extent of response and remediation activities. Therefore, the deployment of an effective, resilient and autonomous radiation monitoring network is pivotal both during and after an incident. Underpinning this assessment is a detailed understanding of the pre-event or background, radiation levels, the knowledge of which is also essential in assessing a population's dosimetric exposure to, and impact from anthropogenic and naturally occurring/varying sources of ionizing radiation. Presented here is a fully operational cloud-based spectroscopic radiation mapping platform comprising IoT modules compatible with cellular networks, without modification, in over 180 countries. Combined with locally roaming vehicles, a continuous multi-pass radiological characterization of an urban environment was performed. Such IoT devices are deployable as either individual sensors for specific localized temporal events or integrated over a greater time period (and area) to represent a larger static sensor. Over several months of continued operation, more than 1000 000 individual location-referenced gamma-ray spectra were collected and securely uploaded, in real-time, to an online cloud database and automatically characterized via a custom multi-step workflow. Fine-scale local variations in the radiological fingerprint of a 1 km × 1 km urban area were subsequently rendered in near-real-time to an interactive secure online graphical dashboard for temporal, spatial and spectral interrogation by the user. Considerations for the automated 'elastic' handling of ever-expanding volumes of input data have been carried out, facilitating propagation and expansion of the system's database without human input.

X-ray nanotomography and electron backscatter diffraction demonstrate the crystalline, heterogeneous and impermeable nature of conodont white matter.

Conodont elements, microfossil remains of extinct primitive vertebrates, are commonly exploited as mineral archives of ocean chemistry, yielding fundamental insights into the palaeotemperature and chemical composition of past oceans. Geochemical assays have been traditionally focused on the so-called lamellar and white matter crown tissues; however, the porosity and crystallographic nature of the white matter and its inferred permeability are disputed, raising concerns over its suitability as a geochemical archive. Here, we constrain the characteristics of this tissue and address conflicting interpretations using ptychographic X-ray-computed tomography (PXCT), pore network analysis, synchrotron radiation X-ray tomographic microscopy (srXTM) and electron back-scatter diffraction (EBSD). PXCT and pore network analyses based on these data reveal that while white matter is extremely porous, the pores are unconnected, rendering this tissue closed to postmortem fluid percolation. EBSD analyses demonstrate that white matter is crystalline and comprised of a single crystal typically tens of micrometres in dimensions. Combined with evidence that conodont elements grow episodically, these data suggest that white matter, which comprises the denticles of conodont elements, grows syntactically, indicating that individual crystals are time heterogeneous. Together these data provide support for the interpretation of conodont white matter as a closed geochemical system and, therefore, its utility of the conodont fossil record as a historical archive of Palaeozoic and Early Mesozoic ocean chemistry.

Miniaturised Low-Cost Gamma Scanning Platform for Contamination Identification, Localisation and Characterisation: A New Instrument in the Decommissioning Toolkit.

Formerly clandestine, abandoned and legacy nuclear facilities, whether associated with civil or military applications, represent a significant decommissioning challenge owing to the lack of knowledge surrounding the existence, location and types of radioactive material(s) that may be present. Consequently, mobile and highly deployable systems that are able to identify, spatially locate and compositionally assay contamination ahead of remedial actions are of vital importance. Deployment imposes constraints to dimensions resulting from small diameter access ports or pipes. Herein, we describe a prototype low-cost, miniaturised and rapidly deployable 'cell characterisation' gamma-ray scanning system to allow for the examination of enclosed (internal) or outdoor (external) spaces for radioactive 'hot-spots'. The readout from the miniaturised and lead-collimated gamma-ray spectrometer, that is progressively rastered through a stepped snake motion, is combined with distance measurements derived from a single-point laser range-finder to obtain an array of measurements in order to yield a 3-dimensional point-cloud, based on a polar coordinate system-scaled for radiation intensity. Existing as a smaller and more cost-effective platform than presently available, we are able to produce a millimetre-accurate 3D volumetric rendering of a space-whether internal or external, onto which fully spectroscopic radiation intensity data can be overlain to pinpoint the exact positions at which (even low abundance) gamma-emitting materials exist.

Sample preparation methods for optimal HS-AFM analysis: Duplex stainless steel.

The contact mode high-speed atomic force microscope (AFM) operates orders of magnitude faster than conventional AFMs. It is capable of capturing multiple frames per second with nanometre-scale lateral resolution and subatomic height resolution. This advancement in imaging rate allows for microscale analysis across macroscale surfaces, making it suitable for applications across materials science. However, the quality of the surface analysis obtained by high-speed AFM is highly dependent upon the standard of sample preparation and the resultant final surface finish. In this study, different surface preparation techniques that are commonly implemented within metallurgical studies are compared for samples of SAF 2205 duplex stainless steel. It was found that, while acid etching and electrolytic etching were optimal for the low resolution of optical microscopy, these methods were less suited for analysis by high resolution high-speed AFM. Mechanical and colloidal silica polishing was found to be the optimal method explored, as it provided a gentle etch of the surface allowing for high quality topographic maps of the sample surface.

Radioactive Source Localisation via Projective Linear Reconstruction.

Radiation mapping, through the detection of ionising gamma-ray emissions, is an important technique used across the nuclear industry to characterise environments over a range of length scales. In complex scenarios, the precise localisation and activity of radiological sources becomes difficult to determine due to the inability to directly image gamma photon emissions. This is a result of the potentially unknown number of sources combined with uncertainties associated with the source-detector separation-causing an apparent 'blurring' of the as-detected radiation field relative to the true distribution. Accurate delimitation of distinct sources is important for decommissioning, waste processing, and homeland security. Therefore, methods for estimating the precise, 'true' solution from radiation mapping measurements are required. Herein is presented a computational method of enhanced radiological source localisation from scanning survey measurements conducted with a robotic arm. The procedure uses an experimentally derived Detector Response Function (DRF) to perform a randomised-Kaczmarz deconvolution from robotically acquired radiation field measurements. The performance of the process is assessed on radiation maps obtained from a series of emulated waste processing scenarios. The results demonstrate a Projective Linear Reconstruction (PLR) algorithm can successfully locate a series of point sources to within 2 cm of the true locations, corresponding to resolution enhancements of between 5× and 10×.

Structural and compositional characteristics of Fukushima release particulate material from Units 1 and 3 elucidates release mechanisms, accident chronology and future decommissioning strategy.

The structural form and elemental distribution of material originating from different Fukushima Daiichi Nuclear Power Plant reactors (Units 1 and 3) is hereby examined to elucidate their contrasting release dynamics and the current in-reactor conditions to influence future decommissioning challenges. Complimentary computed X-ray absorption tomography and X-ray fluorescence data show that the two suites of Si-based material sourced from the different reactor Units have contrasting internal structure and compositional distribution. The known event and condition chronology correlate with the observed internal and external structures of the particulates examined, which suggest that Unit 1 ejecta material sustained a greater degree of melting than that likely derived from reactor Unit 3. In particular, we attribute the near-spherical shape of Unit 1 ejecta and their internal voids to there being sufficient time for surface tension to round these objects before the hot (and so relatively low viscosity) silicate melt cooled to form glass. In contrast, a more complex internal form associated with the sub-mm particulates invoked to originate from Unit 3 suggest a lower peak temperature, over a longer duration. Using volcanic analogues, we consider the structural form of this material and how it relates to its environmental particulate stability and the bulk removal of residual materials from the damaged reactors. We conclude that the brittle and angular Unit 3 particulate are more susceptible to further fragmentation and particulate generation hazard than the round, higher-strength, more homogenous Unit 1 material.

Project Gatekeeper: An Entrance Control System Embedded Radiation Detection Capability for Security Applications.

Threat assessments continue to conclude that terrorist groups and individuals as well as those wanting to cause harm to society have the ambition and increasing means to acquire unconventional weapons such as improvised nuclear explosive devices and radiological disposal devices. Such assessments are given credence by public statements of intent by such groups/persons, by reports of attempts to acquire radioactive material and by law enforcement actions which have interdicted, apprehended or prevented attempts to acquire such material. As a mechanism through which to identify radioactive materials being transported on an individual's person, this work sought to develop a detection system that is of lower-cost, reduced form-factor and more covert than existing infrastructure, while maintaining adequate sensitivity and being retrofittable into an industry standard and widely utilised Gunnebo Speed Gate system. The system developed comprised an array of six off-set Geiger-Muller detectors positioned around the gate, alongside a single scintillator detector for spectroscopy, triggered by the systems inbuilt existing IR proximity sensor. This configuration served to not only reduce the cost for such a system but also allowed for source localisation and identification to be performed. Utilising the current setup, it was possible to detect a 1 µSv/h source carried into the Speed Gate in all test scenarios, alongside locating and spectrally analysing the material in a significant number.

Compositional and structural analysis of Fukushima-derived particulates using high-resolution x-ray imaging and synchrotron characterisation techniques.

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation x-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site - north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume - bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium (134Cs, 135Cs and 137Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.

Radiation Mapping and Laser Profiling Using a Robotic Manipulator.

The use of a robotic arm manipulator as a platform for coincident radiation mapping and laser profiling of radioactive sources on a flat surface is investigated in this work. A combined scanning head, integrating a micro-gamma spectrometer and Time of Flight (ToF) sensor were moved in a raster scan pattern across the surface, autonomously undertaken by the robot arm over a 600 × 260 mm survey area. A series of radioactive sources of different emission intensities were scanned in different configurations to test the accuracy and sensitivity of the system. We demonstrate that in each test configuration the system was able to generate a centimeter accurate 3D model complete with an overlaid radiation map detailing the emitted radiation intensity and the corrected surface dose rate.

Corrigendum: Radiological Mapping of Post-Disaster Nuclear Environments Using Fixed-Wing Unmanned Aerial Systems: A Study From Chornobyl.

[This corrects the article DOI: 10.3389/frobt.2019.00149.].

Evaluation of Scintillator Detection Materials for Application within Airborne Environmental Radiation Monitoring.

In response to the Fukushima Daiichi Nuclear Power Plant accident, there has occurred the unabated growth in the number of airborne platforms developed to perform radiation mapping-each utilising various designs of a low-altitude uncrewed aerial vehicle. Alongside the associated advancements in the airborne system transporting the radiation detection payload, from the earliest radiological analyses performed using gas-filled Geiger-Muller tube detectors, modern radiation detection and mapping platforms are now based near-exclusively on solid-state scintillator detectors. With numerous varieties of such light-emitting crystalline materials now in existence, this combined desk and computational modelling study sought to evaluate the best-available detector material compatible with the requirements for low-altitude autonomous radiation detection, localisation and subsequent high spatial-resolution mapping of both naturally occurring and anthropogenically-derived radionuclides. The ideal geometry of such detector materials is also evaluated. While NaI and CsI (both elementally doped) are (and will likely remain) the mainstays of radiation detection, LaBr3 scintillation detectors were determined to possess not only a greater sensitivity to incident gamma-ray radiation, but also a far superior spectral (energy) resolution over existing and other potentially deployable detector materials. Combined with their current competitive cost, an array of three such composition cylindrical detectors were determined to provide the best means of detecting and discriminating the various incident gamma-rays.

Provenance of uranium particulate contained within Fukushima Daiichi Nuclear Power Plant Unit 1 ejecta material.

Here we report the results of multiple analytical techniques on sub-mm particulate material derived from Unit 1 of the Fukushima Daiichi Nuclear Power Plant to provide a better understanding of the events that occurred and the environmental legacy. Through combined x-ray fluorescence and absorption contrast micro-focused x-ray tomography, entrapped U particulate are observed to exist around the exterior circumference of the highly porous Si-based particle. Further synchrotron radiation analysis of a number of these entrapped particles shows them to exist as UO2-identical to reactor fuel, with confirmation of their nuclear origin shown via mass spectrometry analysis. While unlikely to represent an environmental or health hazard, such assertions would likely change should break-up of the Si-containing bulk particle occur. However, more important to the long-term decommissioning of the reactors at the FDNPP (and environmental clean-upon), is the knowledge that core integrity of reactor Unit 1 was compromised with nuclear material existing outside of the reactors primary containment.

Radiological Mapping of Post-Disaster Nuclear Environments Using Fixed-Wing Unmanned Aerial Systems: A Study From Chornobyl.

In the immediate aftermath following a large-scale release of radioactive material into the environment, it is necessary to determine the spatial distribution of radioactivity quickly. At present, this is conducted by utilizing manned aircraft equipped with large-volume radiation detection systems. Whilst these are capable of mapping large areas quickly, they suffer from a low spatial resolution due to the operating altitude of the aircraft. They are also expensive to deploy and their manned nature means that the operators are still at risk of exposure to potentially harmful ionizing radiation. Previous studies have identified the feasibility of utilizing unmanned aerial systems (UASs) in monitoring radiation in post-disaster environments. However, the majority of these systems suffer from a limited range or are too heavy to be easily integrated into regulatory restrictions that exist on the deployment of UASs worldwide. This study presents a new radiation mapping UAS based on a lightweight (8 kg) fixed-wing unmanned aircraft and tests its suitability to mapping post-disaster radiation in the Chornobyl Exclusion Zone (CEZ). The system is capable of continuous flight for more than 1 h and can resolve small scale changes in dose-rate in high resolution (sub-20 m). It is envisaged that with some minor development, these systems could be utilized to map large areas of hazardous land without exposing a single operator to a harmful dose of ionizing radiation.

Spatial pattern of plutonium and radiocaesium contamination released during the Fukushima Daiichi nuclear power plant disaster.

Plutonium and radiocaesium are hazardous contaminants released by the Fukushima Daiichi nuclear power plant (FDNPP) disaster and their distribution in the environment requires careful characterisation using isotopic information. Comprehensive spatial survey of 134Cs and 137Cs has been conducted on a regular basis since the accident, but the dataset for 135Cs/137Cs atom ratios and trace isotopic analysis of Pu remains limited because of analytical challenges. We have developed a combined chemical procedure to separate Pu and Cs for isotopic analysis of environmental samples from contaminated catchments. Ultra-trace analyses reveal a FDNPP Pu signature in environmental samples, some from further afield than previously reported. For two samples, we attribute the dominant source of Pu to Reactor Unit 3. We review the mechanisms responsible for an emergent spatial pattern in 134,135Cs/137Cs in areas northwest (high 134Cs/137Cs, low 135Cs/137Cs) and southwest (low 134Cs/137Cs, high 135Cs/137Cs) of FDNPP. Several samples exhibit consistent 134,135Cs/137Cs values that are significantly different from those deposited on plant specimens collected in previous works. A complex spatial pattern of Pu and Cs isotopic signature is apparent. To confidently attribute the sources of mixed fallout material, future studies must focus on analysis of individual FDNPP-derived particles.

Development and validation of a high-resolution mapping platform to aid in the public awareness of radiological hazards.

The distribution, quantification and exposure-related effects of radiation in the environment, arising from both natural and anthropogenic sources, is of great (and growing) concern for global populations. Recent events at the Fukushima Daiichi Nuclear Plant (FDNPP) have further highlighted the importance of developing radiation mapping technologies that not only contribute to the continued assessment of contamination, but can serve as an educational tool for members of the public regarding both its behaviour and extent. With an even greater number of people possessing smart-phone technology, a lightweight and portable 'connected system' has been developed to demonstrate to users the calibrated radioactive dose rate in an area, viewable in real-time through a dedicated phone application. As well as allowing for system users to be alerted where variations in dose rate are experienced, the combined results from multiple systems are viewable through a custom-built desktop application-permitting the output obtained via any number of units to be similarly displayed in real-time. A successful initial trialling of the system is described at a former tin mine in Cornwall (south-west England)-known to exhibit low, but identifiable radiation anomalies in discrete areas. Additional applications outside of its educational usage are also discussed.

Feedforward consequences of isometric contractions: effort and ventilation.

The onset of voluntary muscle contractions causes rapid increases in ventilation and is accompanied by a sensation of effort. Both the ventilatory response and perception of effort are proportional to contraction intensity, but these behaviors have been generalized from contractions of a single muscle group. Our aim was to determine how these relationships are affected by simultaneous contractions of multiple muscle groups. We examined the ventilatory response and perceived effort of contraction during separate and simultaneous isometric contractions of the contralateral elbow flexors and of an ipsilateral elbow flexor and knee extensor. Subjects made 10-sec contractions at 25, 50, and 100% of maximum during normocapnia and hypercapnia. For simultaneous contractions, both muscle groups were activated at the same intensities. Ventilation was measured continuously and subjects rated the effort required to produce each contraction. As expected, ventilation and perceived effort increased proportionally with contraction intensity during individual contractions. However, during simultaneous contractions, neither ventilation nor effort reflected the combined muscle output. Rather, the ventilatory response was similar to when contractions were performed separately, and effort ratings showed a small but significant increase for simultaneous contractions. Hypercapnia at rest doubled baseline ventilation, but did not affect the difference in perceived effort between separate and simultaneous contractions. The ventilatory response and the sense of effort at the onset of muscle activity are not related to the total output of the motor pathways, or the working muscles, but arise from cortical regions upstream from the motor cortex.

Altered corticospinal transmission to the hand after maximum voluntary efforts.

INTRODUCTION: After maximal voluntary contractions (MVCs), responses to corticospinal tract stimulation change differently in arm and leg muscles. This study we examined responses in the first dorsal interosseous muscle (FDI). METHODS: Stimulation of the corticospinal tract at the cervicomedullary motor evoked potentials in FDI. Stimuli were delivered before and after 10-s and 1-min MVCs. The reproducibility of changes in the cervicomedullary motor evoked potentials (CMEPs) was investigated. F-waves tested motoneuron excitability. RESULTS: After the MVCs, the CMEP area was initially variable. By ~1 min after 10-s and 1-min MVCs, CMEPs in relaxed muscle decreased to 63 ± 15% and 52 ± 32%, respectively, of control and remained depressed for ~10 min. Responses evoked 2 days apart varied between subjects but not between days. After 10-s MVCs, F-waves were reduced at rest. During weak contraction, CMEPs but not F-waves were depressed. CONCLUSIONS: Our results suggest that contraction produces changes at the corticomotoneuronal synapses to FDI. In addition, motoneuron excitability is reduced.

Long-interval intracortical inhibition in a human hand muscle.

When two motor cortical stimuli are delivered with an interstimulus interval of 50-200 ms, the response (motor evoked potential; MEP) to the second stimulus is typically suppressed. This phenomenon is termed long-interval intracortical inhibition (LICI), although data from one subject suggest that facilitation is possible. Moreover, we recently showed that suppression can be mediated at a spinal level. We characterized LICI more fully by exploring a broad range of contraction strengths and test stimulus intensities. MEPs were evoked in first dorsal interosseous by transcranial magnetic stimulation over the motor cortex. Single test and paired (conditioning-test interval of 100 ms) stimuli at intensities of 100-160% resting motor threshold were delivered at rest or during brief contractions of 10, 25, or 100% maximal voluntary force. Inhibition or facilitation was quantified with the standard ratio in which conditioned MEPs were expressed as a percentage of unconditioned MEPs. Inhibition was greatest at weak-moderate contraction strengths and least at rest and during maximal efforts. Both at rest and during maximal efforts, MEPs evoked by strong stimuli were facilitated. In a subset of subjects, cervicomedullary stimulation was used to activate the corticospinal tract to identify possible spinal influences on changes to MEPs. Contraction strength and test stimulus intensity each had different effects on unconditioned and conditioned MEP size, and hence, LICI is highly dependent on both factors. Further, because motoneurons are facilitated during contraction but disfacilitated after a strong conditioning stimulus, the standard ratio of LICI is of questionable validity during voluntary contractions.