Glacial episodes of a freshwater Arctic Ocean covered by a thick ice shelf.

Following early hypotheses about the possible existence of Arctic ice shelves in the past1-3, the observation of specific erosional features as deep as 1,000 metres below the current sea level confirmed the presence of a thick layer of ice on the Lomonosov Ridge in the central Arctic Ocean and elsewhere4-6. Recent modelling studies have addressed how an ice shelf may have built up in glacial periods, covering most of the Arctic Ocean7,8. So far, however, there is no irrefutable marine-sediment characterization of such an extensive ice shelf in the Arctic, raising doubt about the impact of glacial conditions on the Arctic Ocean. Here we provide evidence for at least two episodes during which the Arctic Ocean and the adjacent Nordic seas were not only covered by an extensive ice shelf, but also filled entirely with fresh water, causing a widespread absence of thorium-230 in marine sediments. We propose that these Arctic freshwater intervals occurred 70,000-62,000 years before present and approximately 150,000-131,000 years before present, corresponding to portions of marine isotope stages 4 and 6. Alternative interpretations of the first occurrence of the calcareous nannofossil Emiliania huxleyi in Arctic sedimentary records would suggest younger ages for the older interval. Our approach explains the unexpected minima in Arctic thorium-230 records9 that have led to divergent interpretations of sedimentation rates10,11 and hampered their use for dating purposes. About nine million cubic kilometres of fresh water is required to explain our isotopic interpretation, a calculation that we support with estimates of hydrological fluxes and altered boundary conditions. A freshwater mass of this size-stored in oceans, rather than land-suggests that a revision of sea-level reconstructions based on freshwater-sensitive stable oxygen isotopes may be required, and that large masses of fresh water could be delivered to the north Atlantic Ocean on very short timescales.

A simple-rapid method to separate uranium, thorium, and protactinium for U-series age-dating of materials.

Uranium-series dating techniques require the isolation of radionuclides in high yields and in fractions free of impurities. Within this context, we describe a novel-rapid method for the separation and purification of U, Th, and Pa. The method takes advantage of differences in the chemistry of U, Th, and Pa, utilizing a commercially-available extraction chromatographic resin (TEVA) and standard reagents. The elution behavior of U, Th, and Pa were optimized using liquid scintillation counting techniques and fractional purity was evaluated by alpha-spectrometry. The overall method was further assessed by isotope dilution alpha-spectrometry for the preliminary age determination of an ancient carbonate sample obtained from the Lake Bonneville site in western Utah (United States). Preliminary evaluations of the method produced elemental purity of greater than 99.99% and radiochemical recoveries exceeding 90% for U and Th and 85% for Pa. Excellent purity and yields (76% for U, 96% for Th and 55% for Pa) were also obtained for the analysis of the carbonate samples and the preliminary Pa and Th ages of about 39,000 years before present are consistent with (14)C-derived age of the material.

Persistent export of 231Pa from the deep central Arctic Ocean over the past 35,000 years.

The Arctic Ocean has an important role in Earth's climate, both through surface processes such as sea-ice formation and transport, and through the production and export of waters at depth that contribute to the global thermohaline circulation. Deciphering the deep Arctic Ocean's palaeo-oceanographic history is a crucial part of understanding its role in climatic change. Here we show that sedimentary ratios of the radionuclides thorium-230 ((230)Th) and protactinium-231 ((231)Pa), which are produced in sea water and removed by particle scavenging on timescales of decades to centuries, respectively, record consistent evidence for the export of (231)Pa from the deep Arctic and may indicate continuous deep-water exchange between the Arctic and Atlantic oceans throughout the past 35,000 years. Seven well-dated box-core records provide a comprehensive overview of (231)Pa and (230)Th burial in Arctic sediments during glacial, deglacial and interglacial conditions. Sedimentary (231)Pa/(230)Th ratios decrease nearly linearly with increasing water depth above the core sites, indicating efficient particle scavenging in the upper water column and greater influence of removal by lateral transport at depth. Although the measured (230)Th burial is in balance with its production in Arctic sea water, integrated depth profiles for all time intervals reveal a deficit in (231)Pa burial that can be balanced only by lateral export in the water column. Because no enhanced sink for (231)Pa has yet been found in the Arctic, our records suggest that deep-water exchange through the Fram strait may export (231)Pa. Such export may have continued for the past 35,000 years, suggesting a century-scale replacement time for deep waters in the Arctic Ocean since the most recent glaciation and a persistent contribution of Arctic waters to the global ocean circulation.

LAFARA: a new underground laboratory in the French Pyrénées for ultra low-level gamma-ray spectrometry.

We describe a new underground laboratory, namely LAFARA (for "LAboratoire de mesure des FAibles RAdioactivités"), that was recently created in the French Pyrénées. This laboratory is primarily designed to analyze environmental samples that display low radioactivity levels using gamma-ray spectrometry. Two high-purity germanium detectors were placed under 85 m of rock (ca. 215 m water equivalent) in the tunnel of Ferrières (Ariège, France). The background is thus reduced by a factor of ∼20 in comparison to above-ground laboratories. Both detectors are fully equipped so that the samples can be analyzed in an automatic mode without requiring permanent presence of a technician in the laboratory. Auto-samplers (twenty positions) and systems to fill liquid nitrogen automatically provide one month of autonomy to the spectrometers. The LAFARA facility allows us to develop new applications in the field of environmental sciences based on the use of natural radionuclides present at low levels in the environment. As an illustration, we present two of these applications: i) dating of marine sediments using the decay of (226)Ra in sedimentary barite (BaSO(4)), ii) determination of (227)Ac ((231)Pa) activities in marine sediment cores.

The determination of absolute intensity of 234mPa's 1001 keV gamma emission using Monte Carlo simulation.

The 1001 keV gamma line of (234m)Pa became important in gamma spectrometric measurements of samples with (238)U content with the advent of development of HpGe detectors of great dimension and high efficiency. In this study the emission probability of the 1001 keV (Y(gamma)) peak of (234m)Pa, was determined by gamma-ray spectrometric measurements performed on glass with Uranium content using Monte Carlo simulation code for efficiency calibration. This method of calculation was not applied for the values quoted in literature so far, at least to our knowledge. The measurements gave an average of 0.836 +/- 0.022%, a value that is in very good agreement to some of the recent results previously presented.

Decay Data Evaluation Project (DDEP): evaluation of the main 233Pa decay characteristics.

The results of a decay data evaluation are presented for 233Pa (beta-) decay to nuclear levels in 233U. These evaluated data have been obtained within the Decay Data Evaluation Project using information published up to 2005.

Measurement of femtogram quantities of protactinium in silicate rock samples by multicollector inductively coupled plasma mass spectrometry.

We describe a new method for the chemical separation and analysis of Pa in silicate rock samples by isotope dilution. Our new technique has the following advantages over previous methods: (a) The initial separation of Pa from the rock matrix is carried out using anionic exchange resin and HCl-HF mixtures, avoiding the need to remove F(-) quantitatively from the sample solution prior to this step, (b) Efficient ionization of Pa is achieved using a multicollector inductively coupled plasma mass spectrometer, so that smaller sample sizes and shorter measurement times are required, compared to previous methods using thermal ionization mass spectrometry or alpha spectrometry. (c) Plasma ionization requires less efficient separation of the high field strength elements from Pa, thus reducing reagent volumes, blanks, and sample preparation times. Instrumental mass fractionation can be corrected for using admixed U of known isotopic composition. Using this method, Pa concentrations can be measured to a precision of approximately 0.5% and an accuracy of approximately 1% using only a few tens of femtograms of Pa.

Analysis of the 237Np-233Pa photon spectrum using the full response function method.

A study has been made of X- and gamma-ray emission from 237Np in equilibrium with 233Pa using the full response function method. This analysis process is characterised by photon spectrometry in which the entire spectrum is modelled in a pseudo-empirical way by means of elementary functions describing the total absorption and escape peaks, the Compton diffusion internal and external to the detector and the peaks resulting from detection of internal conversion electrons. This method has been applied to determine the L X-, K X- and gamma-rays emission probabilities in 237Np and 233Pa decay studies.

A convenient method for discriminating between natural and depleted uranium by gamma-ray spectrometry.

A convenient method for discriminating between natural and depleted uranium reagent was developed by measuring and analyzing the gamma-ray spectra of some reagents with no standard source. The counting rates (R) of photoelectric peaks of gamma-rays from nuclides with the same radioactivity divided by their emission probability (B) are expressed as a function of gamma-ray energy. The radioactivities of 234Th and 234mPa and 21.72 times that of 235U are equal to the radioactivity of 235U in natural uranium. Therefore, the plot of 21.72-fold R/B for 235U should be on a curve fitted to the points for 234Th and 234mPa in natural uranium. Depleted uranium with a 235U isotopic composition of less than 0.68% could be discriminated from natural uranium in the case of a reagent containing 4.0 g of uranium.

Heavy metals and rare earth elements source-sink in some Egyptian cigarettes as determined by neutron activation analysis.

Heavy metals and rare earth elements in two types of cigarettes were studied. The contents of trace elements were determined by using delayed neutron activation analysis. In the present study 11 elements have been detected in popular and fine brand cigarettes marketed in Egypt. Evaluation of these elements with their potential hazards for smokers is briefly discussed. The material balance (source and sink) for each element was determined. Also the ratio of element recovery to the total amount was assessed.

Modelling the contribution of individual radionuclides to the total gamma air kerma rate for the sediments of the Ribble Estuary, NW England.

The aim of this study was to test the performance of a published dose-rate model, investigate the contribution of individual radionuclides to the total gamma air kerma rate (GAKR) and derive external doses to man in the Ribble Estuary, NW England. GAKRs were measured and sediment cores were collected in order to determine radionuclide specific activities with depth. The latter values were used as input data for the external dose-rate model. The model has a slight tendency to over-predict the GAKR, but, on average, the model predictions fall within +/-26% of the measured value. Improvements, in the present case, might be made by accounting for core shortening and variations in soil density in the input data. The model predicted that, for exposed intertidal mud sites, a range of GAKRs between 0.011 and 0.022 microGy h(-1) was attributable to Springfields discharges alone. The contribution due to 234mPa and 234Th ranged between 20 and 60%. An excess GAKR (GAKR arising from anthropogenic emissions alone) of 0.139-0.150 microGy h(-1), used in conjunction with relevant habit-survey data (for a potential critical group) and conversion factors, yielded a dose to man of 0.029-0.031 mSv year(-1).