E. Fourré

3He mass spectrometry for very low-level measurement of organic tritium in environmental samples

The design, setup and performance of a mass spectrometric system for the analysis of low to very low-level tritium in environmental samples are described. The tritium concentration is measured indirectly by the (3)He ingrowth from radioactive decay after complete initial degassing of the sample. The analytical system is fully computer-controlled and consists in a commercial helium isotope mass spectrometer coupled with a high vacuum inlet system. A detection limit of 0.15 Bq/kg is routinely obtainable for sample sizes of 20g of water equivalent and an accumulation time of three months. Larger samples (and/or longer accumulation time) can be used to obtain lower detection limits. In addition to the benefit of a lower detection limit, another advantage of this non-destructive method lies in the simplicity of the analytical procedure which strongly limits the risk of contamination. An inter-comparison was successfully performed with the conventional beta counting technique on lyophilized grass samples, in a range of tritium concentrations of environmental interest. It shows that the (3)He mass spectrometry method yields results that are fully consistent with the conventional liquid scintillation technique over a wide range of tritium concentrations.

Helium isotopes at the Rainbow hydrothermal site (Mid-Atlantic Ridge, 36°14'N)

The 3He/4He ratio and helium concentration have been measured in the vent fluids and the dispersing plume of the Rainbow hydrothermal site, on the Mid-Atlantic Ridge (MAR). The 3He/4He ratio (7.51 Ra) and 3He end-member concentration (25 pmol/kg) are in the range of observed values elsewhere on mid-ocean ridges, pointing to the relative homogeneity of the upper mantle with respect to helium isotope geochemistry. 3He is linearly correlated with methane and manganese throughout the plume, with CH4/3He and Mn/3He ratios identical to those measured in the hot fluids. The bulk residence time of the plume in the rift valley estimated from the plume 3He budget is V20 days. The 3He flux transported by the plume, calculated from current-meter data, is 12.3: 3 nmol/s, requiring a flux of 490 kg/s of high-temperature fluid. The scaling of the heat flux emitted by the Rainbow site to that of 3He, using the 3He/heat ratio measured in the hydrothermal fluids (9.3 :2U10318 mol/J), indicates a heat output of 1320 MW. With a regional spreading rate of V25 mm/year, we calculate that the annual 3He flux for this section of the MAR is of the order of 0.5:0.2 mmol per kilometre of ridge per millimetre of newly formed crust. This figure compares well with the flux calculated for the neighbouring Lucky Strike segment. Although the uncertainties remain large, both fluxes are V40-50% above the world average (0.33 mmol/km/mm), thus supporting earlier suggestions that the intensity of the hydrothermal activity south of the Azores is higher than expected from the regional spreading rate.

Helium transport in sediment pore fluids of the Congo‐Angola margin

During the ZaiRov2 cruise of the ZaiAngo project (1998–2000) on the passive Congo-Angola margin, several gravity cores were analyzed for helium isotopic composition of sedimentary pore waters in two cold fluid seepage zones: the Astrid slide area and the Regab giant pockmark. Gas concentration and isotopic composition are presented along with thermal data in terms of the origin and circulation of fluids. Helium isotope data lie on a mixing line between bottom seawater and an almost pure radiogenic. Helium and temperature vertical profiles are well described by the classic diffusionadvection equation. On the basis of He profiles, we estimate the advection rate on the rim of the pockmark between 1.2 and 2.3 mm/a. The He flux derived for a pure diffusive regime (2.4 × 10 −8 mol/m 2 /a) can favorably be compared to literature data and contrasts with the flux computed close to the pockmark center (1.9 × 10 −7 mol/m 2 /a). Helium depth profiles turned to be more sensitive to advection rate than temperature profiles are.

Oceanic Radiocarbon and Tritium on a Transect between Australia and Bali (Eastern Indian Ocean)

Results are presented of radiocarbon and tritium measurements along a transect between the Australian continental shelf and the Indonesian coast of Bali. The stations lie in the easternmost part of the Indian Ocean, close to the sills over which the Indonesian throughflow (ITF) makes its way to the Indian Ocean. The present data, obtained as part of the Java- Australia Dynamics Experiment (JADE) in August 1989, complement the WOCE 14C and tritium data set on both sides of the Indonesian archipelago and give us the opportunity to discuss the origin of the water masses and timescale of the throughflow. Both tracers point to a north equatorial Pacific origin of the waters. The comparison of the tritium inventories in the Pacific North Equatorial Current and along the JADE transect suggests a minimum transit time of the waters across the Indonesian seaways of the order of 5 to 6 yr, corresponding to a throughflow smaller than 18 106 m3/s.

The distribution of tritium between water and suspended matter in a laboratory experiment exposing sediment to tritiated water.

Following recent suggestions regarding the strong affinity of tritiated water for organic matter in suspended particulates and sediments, two equilibration experiments between sediment organic matter (dry and fresh) and tritiated water were performed to look for potential tritium bio-concentration. The T/H ratios measured at the end of both experiments are lower in the sediment organic matter than in the water, indicating that only a fraction of the hydrogen pool (between 14% and 20%) within the sediment equilibrated with the tritiated water. These results are consistent with the widely used concept of exchangeable and non-exchangeable tritium pools in organic matter and show no sign of tritium bio-accumulation in the sediment relative to water.

Modelling tritium flux from water to atmosphere: application to the Loire River

Tritium (³H or T) is one of the major radionuclides released by nuclear power plants (NPP) into rivers. However, tritiated water (HTO) flux from water to air is seldom considered when assessing health effects of such releases. The aim of this paper is to present the result of a research program, called LORA, conducted on the Loire River (France). To improve our understanding of HTO flux from surface water to air, three field campaigns were organised during the NPPs radioactive releases to measure simultaneously the activity concentrations in air on the riverbank, using an innovative system, and in river water. The measurements showed that during radioactive releases, water vapour was enriched in ³H. These results were used to calibrate exchange velocities. The average of these estimated exchange velocities was more than one order of magnitude higher than those calculated in the literature from indoor experiments. The variability of these values was also larger, showing that outdoor studies cover a wide range of conditions influencing HTO flux. No correlation was observed between exchanges velocities and meteorological conditions. However, there was a significant difference between day and night with a higher value observed during the day. Two approaches used to calculate HTO evaporation from water (i.e. the approach based on water evaporation and the approach considering that HTO follows its own concentration gradient) were included in a hydrodynamic model, which was used to evaluate HTO air activity along the Loire River. In conclusion, only the approach considering that HTO follows its own gradient led to a good agreement between measurements and predictions. A one-year simulation was done to estimate the contribution of this process to the dose. Its contribution can be considered as negligible in this case compared to the other pathways such as ingestion of water or foodstuffs.

Measurement of the French national tritiated-water standard by helium-3 mass spectrometry

The (3)He ingrowth technique is based on the detection of the tritium radioactive daughter, (3)He, by mass spectrometry. Over the last three decades it has been used extensively in oceanography and groundwater studies for measurements of very low to ultra-low levels of tritium. To compare it with the best available methods of radioactive counting, we applied this method to measure the massic activity of a tritiated-water primary standard prepared by the French Laboratoire National Henri Becquerel (LNHB). One liter of a low-level tritium solution was prepared from a small aliquot of the LNHB standard by two-step gravimetric dilution with tritium-free groundwater. Sixteen samples of this solution were analyzed at the LSCE-Saclay noble gas facility, using the (3)He ingrowth method. The massic activity of the prepared solution was also measured by Liquid Scintillation Counting using the Quantulus LNHB counter and an internal calibration method with the LNHB tritiated water standard. All results agree within their standard uncertainty.

Modeling the global bomb tritium transient signal with the AGCM LMDZ‐iso: A method to evaluate aspects of the hydrological cycle

Improving the representation of the hydrological cycle in atmospheric general circulation models (AGCMs) is one of the main challenges in modeling the Earth’s climate system. One way to evaluate model performance is to simulate the transport of water isotopes. Among those available, tritium is an extremely valuable tracer, because its content in the different reservoirs involved in the water cycle (stratosphere, troposphere, and ocean) varies by order of magnitude. Previous work incorporated natural tritium into Laboratoire de Meteorologie Dynamique Zoom (LMDZ)-iso, a version of the LMDZ general circulation model enhanced by water isotope diagnostics. Here for the first time, the anthropogenic tritium injected by each of the atmospheric nuclear bomb tests between 1945 and 1980 has been first estimated and further implemented in the model; it creates an opportunity to evaluate certain aspects of LDMZ over several decades by following the bomb tritium transient signal through the hydrological cycle. Simulations of tritium in water vapor and precipitation for the period 1950–2008, with both natural and anthropogenic components, are presented in this study. LMDZ-iso satisfactorily reproduces the general shape of the temporal evolution of tritium. However, LMDZ-iso simulates too high a bomb tritium peak followed by too strong a decrease of tritium in precipitation. The too diffusive vertical advection in AGCMs crucially affects the residence time of tritium in the stratosphere. This insight into model performance demonstrates that the implementation of tritium in an AGCM provides a new and valuable test of the modeled atmospheric transport, complementing water stable isotope modeling.

3He/4He Ratio in Olivines from Linosa, Ustica, and Pantelleria Islands (Southern Italy)

We report helium isotope data for 0.03–1 Ma olivine-bearing basaltic hawaiites from three volcanoes of the southern Italy magmatic province (Ustica, Pantelleria, and Linosa Islands). Homogenous 3He/4He ratios (range: 7.3–7.6 Ra) for the three islands, and their similarity with the ratio of modern volcanic gases on Pantelleria, indicate a common magmatic end-member. In particular, Ustica (7.6±0.2 Ra) clearly differs from the nearby Aeolian Islands Arc volcanism, despite its location on the Tyrrhenian side of the plate boundary. Although limited in size, our data set complements the large existing database for helium isotope in southern Italy and adds further constraints upon the spatial extent of intraplate alkaline volcanism in southern Mediterranea. As already discussed by others, the He-Pb isotopic signature of this magmatic province indicates a derivation from a mantle diapir of a OIB-type that is partially diluted by the depleted upper mantle (MORB mantle) at its periphery.

High production of H-2 and CH4 and abiotic hydrocarbons in ultramafic-hosted hydrothermal systems on the Mid-Atlantic Ridge

Long abstract only. To assess their relative contributions, geochemical and strontium isotopic analyses were carried out on gas well discharges, groundwater, brines, AMD seeps, and siderite from sedimentary strata.