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.

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.

A performance estimate for the detection of undeclared nuclear-fuel reprocessing by atmospheric 85Kr.

To test the sensitivity of using atmospheric (85)Kr to detect undeclared separation of plutonium from irradiated nuclear-reactor fuel, measurements of atmospheric (85)Kr taken in Tsukuba, Japan are analyzed to determine: (1) a lower limit of detection for discovering anthropogenic (85)Kr emissions, (2) the probability of detecting plutonium separation at the Tokai Reprocessing Plant, and (3) the extent to which these results can be generalized to other sites. A LLD of at least 3.4 sigma=0.14 Bq/m(3) with a theoretical false-positive rate of 0.05% is recommended for safeguards' purposes. At this threshold, the continuous separation of 100, 300, and 900 g equivalent weapon-grade plutonium per day was found to correspond to 10%, 50%, and 80% probability of detection, respectively. The smallest detected concentration was for the continuous separation of 45 g/day, with a probability of detection of about 0.6%. It was found that the detection rate is determined predominantly by the weather.

Simulating mesoscale transport and diffusion of radioactive noble gases using the Lagrangian particle dispersion model.

In order to simulate the impact of mesoscale wind fields and to assess potential capability of atmospheric Lagrangian particle dispersion model (LPDM) as an emergency response model for the decision supports, two different simulations of LPDM with the mesoscale prognostic model MM5 (Mesoscale Model ver. 5) were driven. The first simulation of radioactive noble gas (85Kr exponent) emitted during JCO accident occurred from 30 September to 3 October 1999 at Tokai, Japan showed that the first arriving short pulse was found in Tsukuba located at 60 km away from the accidental area. However, the released radioactive noble gas was transported back to the origin site about 2 days later due to the mesoscale meteorological wind circulation, enhancing the levels of 85Kr with the secondary peak in Tsukuba. The second simulation of atmospheric dilution factors (the ratio of concentration to the emission rate, chi/Q), during the underground nuclear test (UNT) performed by North Korea showed that high chi/Q moved to the eastward and extended toward southward in accordance with the mesoscale atmospheric circulations generated by mesoscale prognostic model MM5. In comparison with the measurements, the simulated horizontal distribution patterns of 85Kr during the JCO are well accord with that of observation in Tsukuba such as the existence of secondary peak which is associated with the mesoscale circulations. However, the simulated level of 85Kr anomaly was found to be significantly lower than the observations, and some interpretations on these discrepancies were described. Applications of LPDM to two mesoscale emergency response dispersion cases suggest the potential capability of LPDM to be used as a decision support model provided accurate emission rate of accident in case of a large accident.

Characterization of two-phase flow regimes in horizontal tubes using 81mKr tracer experiments.

The diagnosis of heat exchangers on duty with respect to flow mal-distributions needs the development of non-intrusive inlet-outlet experimental techniques in order to perform an online fault diagnosis. Tracer experiments are an example of such techniques. They can be applied to mono-phase heat exchangers but also to multi-phase ones. In this case, the tracer experiments are more difficult to perform. In order to check for the capabilities of tracer experiments to be used for the flow mal-distribution diagnosis in the case of multi-phase heat exchangers, we present here a preliminary study on the simplest possible system: two-phase flows in a horizontal tube. (81m)Kr is used as gas tracer and properly collimated NaI (TI) crystal scintillators as detectors. The specific shape of the tracer response allows two-phase flow regimes to be characterized. Signal analysis allows the estimation of the gas phase real average velocity and consequently of the liquid phase real average velocity as well as of the volumetric void fraction. These results are compared successfully to those obtained with liquid phase tracer experiments previously presented by Oriol et al. 2007. Characterization of the two-phase flow regimes and liquid dispersion in horizontal and vertical tubes using coloured tracer and no intrusive optical detector. Chem. Eng. Sci. 63(1), 24-34, as well as to those given by correlations from literature.

A rare combination of cardiopulmonary anomalies demonstrated on ventilation-perfusion scan.

In this case report we describe an unusual appearance seen on a ventilation-perfusion (V/Q) scan in a woman with pulmonary hypertension. Although the pulmonary hypertension was not caused by pulmonary emboli, the V/Q scan suggested several cardiac anomalies which may lead to pulmonary hypertension. Most of the cardiac anomalies, including right-sided aortic arch and right-to-left shunt, can be deduced from careful examination of the V/Q scan. A subsequent cardiac MRI scan confirmed the anomalies.

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.

Coregistered ventilation and perfusion SPECT using krypton-81m and Tc-99m-labeled macroaggregated albumin with multislice CT utility for prediction of postoperative lung function in non-small cell lung cancer patients.

RATIONALE AND OBJECTIVE: Co-registered SPECT and CT imaging (SPECT-CT) has potential for more precise evaluation of regional pulmonary function and may be useful for prediction of postoperative lung function in non-small cell lung cancer (NSCLC) patients. The purpose of the present study was to prospectively assess the capability of co-registered SPECT-CT using krypton-81m (Kr-81m) and technetium-99m-labeled macroaggregated albumin (Tc-99m MAA) for prediction of postoperative lung function of NSCLC patients compared with SPECT and planar imaging. MATERIALS AND METHODS: Sixty consecutive patients considered candidates for lung resection underwent 16-slice CT, ventilation and perfusion scintigraphy with SPECT examinations, and preoperative and postoperative measurement of FEV(1)%. In each subject, SPECT and CT data were automatically fused by using commercially available software. Each postoperative FEV(1)% value was predicted from uptakes of Kr-81m and Tc-99m MAA within total and resected lungs. Then, reproducibility coefficients and the limits of agreement between actual and each predicted postoperative lung function were statistically assessed. RESULTS: Reproducibility coefficients of SPECT-CT (Kr-81m: 5.1%, Tc-99m MAA: 5.2%) were smaller than those of SPECT and planar image using Kr-81m (SPECT: 7.4%, planar image: 12.1%) and using Tc-99m MAA (SPECT: 7.2%, planar image: 11.8%). The limits of agreement for SPECT-CT (Kr-81m: 3.3 +/- 10.5%, Tc-99m MAA: 5.4 +/- 11.0%) were also smaller than that of SPECT and planar image and small enough for clinical purposes. CONCLUSIONS: Co-registered SPECT-CT using Kr-81m and Tc-99m MAA was able to more reproducibly and accurately predict postoperative lung function compared with SPECT and planar imaging.

Noble gas radionuclides in RBMK-1500-type reactor.

The presence of noble gas and other short-lived radionuclides in air borne effluents from RBMK-1500-type reactor has been investigated using experimental and theoretical instrumentation for detection purposes. Activity concentrations of (85m)Kr, (87)Kr, (88)Kr, (135m)Xe, (135)Xe, (133)Xe and (41)Ar were measured in air emissions from Ignalina NPP using a special method and special equipment. Theoretical detection of reactor-borne radionuclides and investigation of their behaviour in a nuclear fuel during operation of nuclear reactor was performed using an analytical model based on reactor physics. An innovative method for the estimation of noble gas flow time from the defective nuclear fuel element through the ventilation stack of NPP to the atmosphere based on comparison of the experimentally and theoretically evaluated activity ratios of (88)Kr/(85m)Kr; (135)Xe/(133)Xe has been proposed. The estimated flow time of noble gas provides an excellent possibility to obtain modelling-based information about the qualitative and quantitative content of atmospheric releases from NPP.

On-site gamma-ray spectroscopic measurements of fission gas release in irradiated nuclear fuel.

An experimental, non-destructive in-pool, method for measuring fission gas release (FGR) in irradiated nuclear fuel has been developed. Using the method, a significant number of experiments have been performed in-pool at several nuclear power plants of the BWR type. The method utilises the 514 keV gamma-radiation from the gaseous fission product (85)Kr captured in the fuel rod plenum volume. A submergible measuring device (LOKET) consisting of an HPGe-detector and a collimator system was utilised allowing for single rod measurements on virtually all types of BWR fuel. A FGR database covering a wide range of burn-ups (up to average rod burn-up well above 60 MWd/kgU), irradiation history, fuel rod position in cross section and fuel designs has been compiled and used for computer code benchmarking, fuel performance analysis and feedback to reactor operators. Measurements clearly indicate the low FGR in more modern fuel designs in comparison to older fuel types.

Characteristics of a 85Kr beta-particle source applied in Series 1 reference irradiations of DIS-1 direct ion storage dosemeters.

Characteristics necessary to specify an ISO 6980 Series 1 reference radiation field were determined for a commercially available 85Kr beta-particle source, using a BEAM EGS4 Monte Carlo code. The characteristics include residual maximum beta energy, E(res), and the uniformity of the dose rate over the calibration area. The E(res) and the uniformity were also determined experimentally, using an extrapolation ionization chamber (EC) and a 0.2 cm3 parallel plate ionization chamber, respectively. The depth-dose curve measured with the EC gave a value 0.62 MeV for the E(res). Series 2 90Sr + 90Y and Series 1(85) Kr beta-particle sources calibrated for H(p)(0.07) at the secondary standard dosimetry laboratory (SSDL) of STUK were used to determine the energy and angular responses of DIS-1 direct ion storage dosemeters. The averaged zero angle H(p)(0.07) responses to the 90Sr + 90Y and 85Kr reference radiations were 135 and 80%, respectively. The responses were normalized to 100%, H(p)(0.07) response to 137Cs photon radiation.

Comparative analysis of different scintigraphic approaches to assess pulmonary ventilation.

A study was carried out to investigate the predictive value of 81-metastable-krypton (81mKr) distribution, high-size 99-metastable-technetium (99mTc) aerosol deposition and low-size 99mTc aerosol (Technegas) deposition on the pulmonary ventilation evaluated by 133-xenon (133Xe) lung scintigraphy, and to assess the correlation between the 81mKr distribution, the 99mTc aerosols deposition, and the respiratory parameters of patients with chronic obstructive pulmonary disease (COPD). Twenty COPD patients were included. The 81mKr, 133Xe, and 99mTc aerosol lung scintigraphies were successively carried out. The 81mKr distribution and 99mTc deposition were compared to the 133Xe distribution at equilibrium and to the 133Xe clearance. Sensitivity, specificity, positive predictive value (PPV), and negative predictive value (NPV) of 81mKr and Technegas lung scintigraphies to detect alterations in ventilation revealed by 133Xe were defined. The 81mKr distribution and 99mTc deposition according to respiratory parameters were described using a principal component analysis. Compared to 133Xe distribution, a significantly higher distribution of 81mKr in the upper parts of the lungs in the more severe patients (p = 0.05), a significantly higher deposition of Technegas in the lower parts of the lungs (p = 0.0008), and a significantly higher deposition in the central parts of the high-size 99mTc aerosol were observed (p = 0.0001). The PPV and the NPV were, respectively, 0.54 and 0.58 for 81mKr and 0.54 and 0.55 for Technegas. There was a significant negative correlation between 81mKr distribution and 133Xe clearance (p = 0.0001) between Technegas deposition and 133Xe clearance (p = 0.0007), and between 99mTc diethylene-triamino-penta-acetate (DTPA) deposition and 133Xe clearance (p = 0.001). Both the 81mKr peripheral distribution and Technegas peripheral deposition correlated negatively with increased obstruction, as measured by forced expiratory volume in 1 sec (FEV1). Peripheral deposition of the high-size 99mTc aerosol deposition correlated with the inspiration/expiration time ratio. In conclusion, 81mKr and 99mTc aerosols' lung scintigraphies do not reflect exactly the pulmonary ventilation as measured by 133Xe scintigraphy.

Apparent 85Kr ages of groundwater within the Royal watershed, Maine, USA.

Specific 85Kr activity is mapped from 264 domestic and municipal wells sampled during 2002-2004 in the Royal watershed (361 km2), Maine. Gas samples are collected at 20 m, 40 m, and > 50 m interval depths within the unconfined aquifers. Gas extraction for 85Kr from wells is obtained directly via a wellhead methodology avoiding conventional collection of large sample volumes. Atmospheric 85Kr input to the recharge environment is estimated at 1.27 Bq m(-3) by time-series analyses of weighted monthly precipitation (2001-2004). Numerical simulation of Kr gas transport through the variable unsaturated zones to the water table suggests up to 12-year time lags locally, thus biasing the 85Kr groundwater ages. Apparent 85Kr ages suggest that approximately 70% of groundwater near 20 m depth was recharged less than 30 years BP (2004). Mass-age transport modeling suggests that post mid-1950s recharge penetrates to part of the basin's floor and that older groundwater seeps from the underlying fractured bedrock may occur.

Kr-81m calibration factor for the npl ionisation chamber.

A general method has been developed for the measurement of the activity concentration of 81mKr gas. Due to its short half-life, 13.1s, this gas has to be eluted from a 81Rb/81mKr generator. The 81Rb parent has a half-life of about 4.6 h. The calibration was done in two steps: firstly, a gamma-ray spectrometer was calibrated using 51Cr and 139Ce sources, nuclides with gamma-ray energies bracketing that of 81mKr (190.5 keV). The measurement geometry was equivalent to that of the 81mKr measurement; the sources were inserted into two collimated PTFE tubes in front of the gamma-ray detector. Secondly, a calibration factor for the NPL radionuclide calibrator was determined with a specially designed ionisation chamber insert. The 81mKr gas passed in front of the gamma-ray detector in PTFE tubing before and after entering the ionisation chamber. The calibration factor for 81mKr in the radionuclide calibrator with this geometry was independent of the gas flow rate within determined limits. The analytical calculations of the activity determination, uncertainties and measurement criteria are discussed.