Monitoring atmospheric 85Kr by atom counting.

Radioactive 85Kr is a major gaseous fission product emitted into the air by the nuclear fuel reprocessing industry. Measuring atmospheric 85Kr has applications in environmental monitoring, atmospheric transport model validation and dating of environmental water samples, including groundwater, sea water and glacier ice. We present an ultra-sensitive method for fast analysis of atmospheric 85Kr at 10-5 parts per trillion level. This method is based on laser cooling and trapping and is capable of counting individual 85Kr atoms. Measurements at the 3% precision level can be made on krypton extracted from 1L STP of air with a turnaround time of 1.5 h. Moreover, we have realized a system for continuous air sampling over days to weeks. Based on this atom-counting technology and a portable air sample integrator we have realized atmospheric 85Kr baseline monitoring in Hefei, China, for over 20 months. The technological advances presented in this work lay the ground for a global atmospheric 85Kr monitoring network.

Evaluating 5 decades of atmospheric 85Kr measurements in the southern hemisphere to derive an input function for dating water and ice with implications for interhemispheric circulation and the global 85Kr emission inventory.

In July 2015, the currently only active monitoring station for atmospheric 85Kr measurements in the southern hemisphere went operational at the Commonwealth Scientific and Industrial Research Organization (CSIRO) in Adelaide, Australia. Here, this new data is presented and combined with measurements from historic monitoring stations, to generate a85Kr input function for the southern hemisphere which is crucial for the application of 85Kr as a dating tracer for water and ice. After a linear increase in atmospheric 85Kr concentrations between 1980 and 2005, concentrations stabilized yielding mean 85Kr activity concentration during the Adelaide monitoring period of 1.3 ± 0.15 Bq/m³ air with slight variations indicating seasonal effects. Data from three northern hemispheric monitoring stations Schauinsland, Freiburg and Jungfraujoch of the German Federal Office for Radiation Protection (BfS), located in Central Europe are used to calculate an interhemispheric exchange time of 1.25 ± 0.24 years, using a simple box model approach. Furthermore, it is investigated whether a southern hemispheric 85Kr input function can be calculated from the baseline of the northern hemispheric data set. A comparison between the calculated and the fitted input function shows that analytical techniques can just resolve the concentration differences, emphasising the need of southern hemispheric monitoring stations for 85Kr. Analysing the decay-corrected input function and taking the current detection limit of low-level counting and Atom Trap Trace Analysis of 0.05 Bq/m³ air, a maximum apparent 85Kr tracer age of 40 years can be determined in the southern hemisphere. Finally, the 85Kr measurements are used to derive global 85Kr emission rates which are found to be in good agreement with published emissions from nuclear reprocessing plants.

Using isotope data to characterize and date groundwater in the southern sector of the Guaraní Aquifer System.

The Guaraní Aquifer System (SAG) is the largest transboundary aquifer in Latin America, extending beneath parts of Brazil, Paraguay, Argentina, and Uruguay. This paper presents the results of recent hydrogeological studies in the southern portion of the SAG. Locally, the abundance of surface water bodies precluded the use of conventional hydrological tools to characterize groundwater flows. Geological, hydrochemical and environmental isotope investigations were integrated to postulate a revised hydrogeological conceptual model. The revised geological model has provided a better definition of the geometry of the aquifer units and outlined the relevance of regional faults in controlling flow patterns. The new potentiometric map is consistent with groundwater flow from the SAG outcrops to the centre of the Corrientes Province, where upwards flows were identified. Hydrochemical and isotope data confirmed the widespread occurrence of mixing. Noble gas isotopes dissolved in groundwater (4He and 81Kr/Kr) provided residence times ranging from recent recharge up to 770 ± 130 ka. Groundwater age modelling confirmed the role of the geological structures in controlling groundwater flow. The southern sector of the SAG is a multilayer aquifer system with vertical flows and deep regional discharge near the Esteros del Iberá wetland area and along the Paraná and Uruguay rivers.

Half a century of Krypton-85 activity concentration measured in air over Central Europe: Trends and relevance for dating young groundwater.

For almost half a century weekly samples for the measurement of krypton-85 (85Kr) activity concentrations in surface air have been collected by the Bundesamt für Strahlenschutz (BfS), Germany. Sampling started at Freiburg (230m asl) in 1973, Mt Schauinsland (1205m asl) in 1976 and Mt Jungfraujoch in Switzerland (3454 asl) in 1990. Distinct maxima in the time series of atmospheric 85Kr activity concentration are caused by emissions from nuclear reprocessing plants in Europe, mainly the La Hague, France, and Sellafield, UK, reprocessing plants. Between 1970 and 1990 peak activity concentrations measured in winter along the Rhine Rift in Freiburg are often higher than at Mt Schauinsland, due to emissions from the operating pilot reprocessing plant in Karlsruhe - approximately 130 km to the north - and large-scale inversions that inhibit exchange of air masses within the Rhine Rift with those at higher altitudes. From the early 1990s onwards, after the shut-down of the pilot plant, differences between Freiburg and Schauinsland are much smaller. Activity concentrations measured at Jungfraujoch are generally lower and close to baseline levels, due to its location in the free troposphere. Weekly baseline and average 85Kr activity concentration in the atmosphere in Central Europe were modelled from almost 12,000 individual measurements at 11 stations. The baseline and average have continuously increased, interrupted by a relatively stable period between 2009 and the end of 2014 with a baseline activity concentration of about 1.39 Bq/m3. Depending on the geographical location and hydrological conditions, the modelled baseline or average 85Kr activity concentration time series can be used as input functions for the dating of young groundwater.

Simulating the mesoscale transport of krypton-85.

Due to its half-life, chemical inertness and low solubility in water, radioactive 85Kr is a valuable tracer for testing the performance of atmospheric dispersion models in simulating long-range transport of pollutants. This paper evaluates the capability of simulating the dispersion of radiokrypton emitted by a nuclear fuel reprocessing plant in north-west France. Three time periods during which elevated activity concentrations of 85Kr in ground level air were detected in south-west Germany are chosen. Simulations have been performed using the HYSPLIT code and the European Centre for Median-Range Weather Forecasts (ECMWF) data base. Although their results show a slight trend of underestimating the measured 85Kr concentrations, there is a significant correlation and moderate scatter between observations and simulations with about 50% of the results being within a factor of two of the measured concentrations. The simulated travel time distributions provided a valuable tool for providing additional insight into the dispersion of the tracer radionuclides and for identifying potential causes of deviations between measured and calculated concentrations.

MCNPX CALCULATIONS OF SPECIFIC ABSORBED FRACTIONS IN SOME ORGANS OF THE HUMAN BODY DUE TO APPLICATION OF 133Xe, 99mTc and 81mKr RADIONUCLIDES.

Monte Carlo simulations were performed to evaluate treatment doses with wide spread used radionuclides 133Xe, 99mTc and 81mKr. These different radionuclides are used in perfusion or ventilation examinations in nuclear medicine and as indicators for cardiovascular and pulmonary diseases. The objective of this work was to estimate the specific absorbed fractions in surrounding organs and tissues, when these radionuclides are incorporated in the lungs. For this purpose a voxel thorax model has been developed and compared with the ORNL phantom. All calculations and simulations were performed by means of the MCNP5/X code.

Present and future potential of krypton-85 for the detection of clandestine reprocessing plants for treaty verification.

Burnup calculations are applied to determine the amount of krypton-85 that is produced during the irradiation of nuclear fuel. Since krypton-85 is most likely released into the atmosphere during reprocessing to separate plutonium, atmospheric transport modeling is used to calculate the worldwide distribution of krypton-85 concentrations stemming from emissions from declared reprocessing plants. The results are the basis for scenarios in which emissions from clandestine reprocessing facilities have to be detected against various background levels. It is concluded that today's background imposes heavily on the ability to detect small and medium plutonium separation rates; only high separation rates of 1 SQ per week and higher have a chance to be detected with feasible outlay. A fixed network of monitoring stations seems too costly; instead the high number of samples that are required rather calls for mobile sampling procedures, where air samples are collected at random locations over the world and are analyzed in regional laboratories for their krypton-85 concentration. Further, it is argued that krypton-85 emissions from declared reprocessing activities have to be significantly lowered to enable a worldwide verification of the absence of even smaller clandestine reprocessing. For each scenario the number of samples that have to be taken for probable detection is calculated.

Evaluation of four-dimensional computed tomography (4D-CT)-based pulmonary ventilation: The high correlation between 4D-CT ventilation and (81m)Kr-planar images was found.

PURPOSE: To evaluate four-dimensional computed tomography (4D-CT)-derived pulmonary ventilation by comparing with (81m)Kr-gas ventilation (VRI). We also proposed two methods to improve the functional accuracy of 4D-CT ventilation images and evaluated these methods. METHODS AND MATERIALS: Eleven lung cancer patients with 4D-CT and VRI were analyzed. Hounsfield unit-based (VHU) and a Jacobian-based (VJac) 4D-CT ventilation images were calculated. They were evaluated by voxel-by-voxel spearman's rank correlation coefficient (r) between 4D-CT ventilation and VRI images. After applying an averaging ventilation method and a slope calculating method, correlations were also calculated. RESULTS: 4D-CT ventilation showed the high correlation to VRI (r=0.875 with VHU). An averaging method brought significantly higher (p=0.012) correlations to nuclear medicine images with VHU. The improvement was not significant (p=0.619) with VJac. Slope calculating method improved the correlation with VHU and slightly worsened the correlation with VJac. CONCLUSIONS: The averaging method we proposed might be useful to improve 4D-CT ventilation images. We found good agreement between 4D-CT ventilation and nuclear medicine ventilation, indicating the high physiologic accuracy of 4D-CT ventilation.

Impact of acoustic airflow on intrasinus drug deposition: New insights into the vibrating mode and the optimal acoustic frequency to enhance the delivery of nebulized antibiotic.

AIM: We investigated the impact of vibrating acoustic airflow, the high frequency (f≥100 Hz) and the low frequency (f≤45 Hz) sound waves, on the enhancement of intrasinus drug deposition. METHODS: (81m)Kr-gas ventilation study was performed in a plastinated human cast with and without the addition of vibrating acoustic airflow. Similarly, intrasinus drug deposition in a nasal replica using gentamicin as a marker was studied with and without the superposition of different modes of acoustic airflow. RESULTS: Ventilation experiments demonstrate that no sinus ventilation was observed without acoustic airflow although sinus ventilation occurred whatever the modes of acoustic airflow applied. Intrasinus drug deposition experiments showed that the high frequency acoustic airflow led to 4-fold increase in gentamicin deposition into the left maxillary sinus and to 2-fold deposition increase into the right maxillary sinus. Besides, the low frequency acoustic airflow demonstrated a significant increase of 4-fold and 2-fold in the right and left maxillary sinuses, respectively. CONCLUSION: We demonstrated the benefit of different modes of vibrating acoustic airflow for maxillary sinus ventilation and intrasinus drug deposition. The degree of gentamicin deposition varies as a function of frequency of the vibrating acoustic airflow and the geometry of the ostia.

Estimation of 85Kr dispersion from the spent nuclear fuel reprocessing plant in Rokkasho, Japan, using an atmospheric dispersion model.

The spent nuclear fuel reprocessing plant of Japan Nuclear Fuel Limited (JNFL) located in Rokkasho, Japan, discharged small amounts of (85)Kr into the atmosphere during final tests of the plant with actual spent fuel from 31 March 2006 to October 2008. During this period, the gamma-ray dose rates due to discharged (85)Kr were higher than the background rates measured at the Institute for Environmental Sciences and at seven monitoring stations of the Aomori prefectural government and JNFL. The dispersion of (85)Kr was simulated by means of the fifth-generation Penn State/NCAR Mesoscale Model and the CG-MATHEW/ADPIC models (ver. 5.0) with a vertical terrain-following height coordinate. Although the simulated gamma-ray dose rates due to discharged (85)Kr agreed fairly well with measured rates, the agreement between the estimated monthly mean (85)Kr concentrations and the observed concentrations was poor. Improvement of the vertical flow of air may lead to better estimation of (85)Kr dispersion.

Nasal high flow clears anatomical dead space in upper airway models.

Recent studies showed that nasal high flow (NHF) with or without supplemental oxygen can assist ventilation of patients with chronic respiratory and sleep disorders. The hypothesis of this study was to test whether NHF can clear dead space in two different models of the upper nasal airways. The first was a simple tube model consisting of a nozzle to simulate the nasal valve area, connected to a cylindrical tube to simulate the nasal cavity. The second was a more complex anatomically representative upper airway model, constructed from segmented CT-scan images of a healthy volunteer. After filling the models with tracer gases, NHF was delivered at rates of 15, 30, and 45 l/min. The tracer gas clearance was determined using dynamic infrared CO2 spectroscopy and 81mKr-gas radioactive gamma camera imaging. There was a similar tracer-gas clearance characteristic in the tube model and the upper airway model: clearance half-times were below 1.0 s and decreased with increasing NHF rates. For both models, the anterior compartments demonstrated faster clearance levels (half-times < 0.5 s) and the posterior sections showed slower clearance (half-times < 1.0 s). Both imaging methods showed similar flow-dependent tracer-gas clearance in the models. For the anatomically based model, there was complete tracer-gas removal from the nasal cavities within 1.0 s. The level of clearance in the nasal cavities increased by 1.8 ml/s for every 1.0 l/min increase in the rate of NHF. The study has demonstrated the fast-occurring clearance of nasal cavities by NHF therapy, which is capable of reducing of dead space rebreathing.

Near-field krypton-85 measurements in stable meteorological conditions around the AREVA NC La Hague reprocessing plant: estimation of atmospheric transfer coefficients.

The aim of this work was to study the near-field dispersion of (85)Kr around the nuclear fuel reprocessing plant at La Hague (AREVA NC La Hague - France) under stable meteorological conditions. Twenty-two (85)Kr night-time experimental campaigns were carried out at distances of up to 4 km from the release source. Although the operational Gaussian models predict for these meteorological conditions a distance to plume touchdown of several kilometers, we almost systematically observed a marked ground signal at distances of 0.5-4 km. The calculated atmospheric transfer coefficients (ATC) show values (1) higher than those observed under neutral conditions, (2) much higher than those proposed by the operational models, and (3) higher than those used in the impact assessments.

Radiometric 81Kr dating identifies 120,000-year-old ice at Taylor Glacier, Antarctica.

We present successful (81)Kr-Kr radiometric dating of ancient polar ice. Krypton was extracted from the air bubbles in four ∼350-kg polar ice samples from Taylor Glacier in the McMurdo Dry Valleys, Antarctica, and dated using Atom Trap Trace Analysis (ATTA). The (81)Kr radiometric ages agree with independent age estimates obtained from stratigraphic dating techniques with a mean absolute age offset of 6 ± 2.5 ka. Our experimental methods and sampling strategy are validated by (i) (85)Kr and (39)Ar analyses that show the samples to be free of modern air contamination and (ii) air content measurements that show the ice did not experience gas loss. We estimate the error in the (81)Kr ages due to past geomagnetic variability to be below 3 ka. We show that ice from the previous interglacial period (Marine Isotope Stage 5e, 130-115 ka before present) can be found in abundance near the surface of Taylor Glacier. Our study paves the way for reliable radiometric dating of ancient ice in blue ice areas and margin sites where large samples are available, greatly enhancing their scientific value as archives of old ice and meteorites. At present, ATTA (81)Kr analysis requires a 40-80-kg ice sample; as sample requirements continue to decrease, (81)Kr dating of ice cores is a future possibility.

Krypton-81 in groundwater of the Culebra Dolomite near the Waste Isolation Pilot Plant, New Mexico.

The Waste Isolation Pilot Plant (WIPP) in New Mexico is the first geologic repository for disposal of transuranic nuclear waste from defense-related programs of the US Department of Energy. It is constructed within halite beds of the Permian-age Salado Formation. The Culebra Dolomite, confined within Rustler Formation evaporites overlying the Salado Formation, is a potential pathway for radionuclide transport from the repository to the accessible environment in the human-disturbed repository scenario. Although extensive subsurface characterization and numerical flow modeling of groundwater has been done in the vicinity of the WIPP, few studies have used natural isotopic tracers to validate the flow models and to better understand solute transport at this site. The advent of Atom-Trap Trace Analysis (ATTA) has enabled routine measurement of cosmogenic (81)Kr (half-life 229,000 yr), a near-ideal tracer for long-term groundwater transport. We measured (81)Kr in saline groundwater sampled from two Culebra Dolomite monitoring wells near the WIPP site, and compared (81)Kr model ages with reverse particle-tracking results of well-calibrated flow models. The (81)Kr model ages are ~130,000 and ~330,000 yr for high-transmissivity and low-transmissivity portions of the formation, respectively. Compared with flow model results which indicate a relatively young mean hydraulic age (~32,000 yr), the (81)Kr model ages imply substantial physical attenuation of conservative solutes in the Culebra Dolomite and provide limits on the effective diffusivity of contaminants into the confining aquitards.

Variability of atmospheric krypton-85 activity concentrations observed close to the ITCZ in the southern hemisphere.

Krypton-85 activity concentrations in surface air have been measured at Darwin, which is located in northern Australia and is influenced by seasonal monsoonal activity. Measurements between August 2007 and May 2010 covered three wet seasons. The mean activity concentration of krypton-85 measured during this period was 1.31±0.02Bqm(-3). A linear model fitted to the average monthly data, using month and monsoon as predictors, shows that krypton-85 activity concentration measured during the sampling period has declined by 0.01Bqm(-3) per year. Although there is no statistically significant difference in mean activity concentration of krypton-85 between wet and dry season, the model implies that activity concentration is higher by about 0.015Bqm(-3) during months influenced by the monsoon when a north westerly flow prevails. Backward dispersion runs using the Lagrangian particle dispersion model Hysplit4 highlight possible source regions during an active monsoon located deep in the northern hemisphere, and include reprocessing facilities in Japan and India. However, the contribution of these facilities to krypton-85 activity concentrations in Darwin would be less than 0.003Bqm(-3).

Monte Carlo modelling of 90Sr/90Y and 85Kr beta fields for Hp(3) measurements.

In support of research aimed at developing a thermoluminescence dosemeter capable of accurately measuring ionising radiation doses to the lens of the eye, Monte Carlo modelling of a standard beta exposure set-up has been performed. It was found that electrons with an energy distribution corresponding to the beta emission spectrum from (85)Kr deposit negligible doses at a depth of 3 mm in tissue, but doses from (90)Sr/(90)Y are significant; free in air and fluence-to-Hp(3,θ°) and -Hp(0.07,θ°) conversion coefficient data were found for this field for exposures at 0°, 30° and 60° angles of incidence, and the response characteristics of the new eye dosemeter were evaluated. It was shown that the results were not affected greatly by the shape of the calibration phantom. However, it was demonstrated that the presence of intermediating air and beam flattening filters hardens the energy distribution of the field at the point of test, relative to a raw (90)Sr/(90)Y source, and this impacts dose depositions.

Comparison of RIMPUFF, HYSPLIT, ADMS atmospheric dispersion model outputs, using emergency response procedures, with (85)Kr measurements made in the vicinity of nuclear reprocessing plant.

The Institut de Radioprotection et de Sureté Nucléaire (IRSN) performed a series of (85)Kr air sampling campaigns at mesoscale distances (18-50 km) from the AREVA NC La Hague nuclear reprocessing plant (North West France) between 2007 and 2009. The samples were collected in order to test and optimise a technique to measure low krypton-85 ((85)Kr) air concentrations and to investigate the performance of three atmospheric dispersion models (RIMPUFF, HYSPLIT, and ADMS), This paper presents the (85)Kr air concentrations measured at three sampling locations which varied from 2 to 8000 Bq m(-3), along with the (85)Kr air concentrations output by the dispersion models. The dispersion models made reasonable estimates of the mean concentrations of (85)Kr field measurements during steady wind conditions. In contrast, the models failed to accurately predict peaks in (85)Kr air concentration during periods of rapid and large changes in wind speed and/or wind direction. At distances where we made the comparisons (18-50 km), in all cases, the models underestimated the air concentration activities.

Analysis of 85Kr: a comparison at the 10 -14 level using micro-liter samples.

The isotopic abundance of (85)Kr in the atmosphere, currently at the level of 10(-11), has increased by orders of magnitude since the dawn of nuclear age. With a half-life of 10.76 years, (85)Kr is of great interest as tracers for environmental samples such as air, groundwater and ice. Atom Trap Trace Analysis (ATTA) is an emerging method for the analysis of rare krypton isotopes at isotopic abundance levels as low as 10(-14) using krypton gas samples of a few micro-liters. Both the reliability and reproducibility of the method are examined in the present study by an inter-comparison among different instruments. The (85)Kr/Kr ratios of 12 samples, in the range of 10(-13) to 10(-10), are measured independently in three laboratories: a low-level counting laboratory in Bern, Switzerland, and two ATTA laboratories, one in Hefei, China, and another in Argonne, USA. The results are in agreement at the precision level of 5%.