Noble gas, CFC and other geochemical evidence for the age and origin of the Bath thermal waters, UK

The city of Bath is a World Heritage site and its thermal waters, the Roman Baths and new spa development rely on undisturbed flow of the springs (45 °C). The current investigations provide an improved understanding of the residence times and flow regime as basis for the source protection. Trace gas indicators including the noble gases (helium, neon, argon, krypton and xenon) and chlorofluorocarbons (CFCs), together with a more comprehensive examination of chemical and stable isotope tracers are used to characterise the sources of the thermal water and any modern components. It is shown conclusively by the use of 39Ar that the bulk of the thermal water has been in circulation within the Carboniferous Limestone for at least 1000 years. Other stable isotope and noble gas measurements confirm previous findings and strongly suggest recharge within the Holocene time period (i.e. the last 12 kyr). Measurements of dissolved 85Kr and chlorofluorocarbons constrain previous indications from tritium that a small proportion (<5%) of the thermal water originates from modern leakage into the spring pipe passing through Mesozoic valley fill underlying Bath. This introduces small amounts of O2 into the system, resulting in the Fe precipitation seen in the King’s Spring. Silica geothermometry indicates that the water is likely to have reached a maximum temperature of between 69–99 °C, indicating a most probable maximum circulation depth of ∼3 km, which is in line with recent geological models. The rise to the surface of the water is sufficiently indirect that a temperature loss of >20 °C is incurred. There is overwhelming evidence that the water has evolved within the Carboniferous Limestone formation, although the chemistry alone cannot pinpoint the geometry of the recharge area or circulation route. For a likely residence time of 1–12 kyr, volumetric calculations imply a large storage volume and circulation pathway if typical porosities of the limestone at depth are used, indicating that much of the Bath-Bristol basin must be involved in the water storage.

Light noble gases in 12 meteorites from the Omani desert, Australia, Mauritania, Canada, and Sweden

We measured the concentrations and isotopic compositions of He, Ne, and Ar in 14 fragments from 12 different meteorites: three carbonaceous chondrites, six L chondrites (three most likely paired), one H chondrite, one R chondrite, and one ungrouped chondrite. The data obtained for the CV3 chondrites Ramlat as Sahmah (RaS) 221 and RaS 251 support the hypothesis of exposure age peaks for CV chondrites at approximately 9 Ma and 27 Ma. The exposure age for Shişr 033 (CR chondrite) of 7.3 Ma is also indicative of a possible CR chondrite exposure age peak. The three L chondrites Jiddat al Harasis (JaH) 091, JaH 230, and JaH 296, which are most likely paired, fall together with Hallingeberg into the L chondrite exposure age peak of approximately 15 Ma. The two L chondrites Shelburne and Lake Torrens fall into the peaks at approximately 40 Ma and 5 Ma, respectively. The ages for Bassikounou (H chondrite) and RaS 201 (R chondrite) are approximately 3.5 Ma and 5.8 Ma, respectively. Six of the studied meteorites show clear evidence for 3He diffusive losses, the deficits range from approximately 17% for one Lake Torrens aliquot to approximately 45% for RaS 211. The three carbonaceous chondrites RaS 221, RaS 251, and Shişr 033 all have excess 4He, either of planetary or solar origin. However, very high 4He/20Ne ratios occur at relatively low 20Ne/22Ne ratios, which is unexpected and needs further study. The measured 40Ar ages fit well into established systematics. They are between 2.5 and 4.5 Ga for the carbonaceous chondrites, older than 3.6 Ga for the L and H chondrites, and about 2.4 Ga for the R chondrite as well as for the ungrouped chondrite. Interestingly, none of our studied L chondrites has been degassed in the 470 Ma break-up event. Using the amount of trapped 36Ar as a proxy for noble gas contamination due to terrestrial weathering we are able to demonstrate that the samples studied here are not or only very slightly affected by terrestrial weathering (at least in terms of their noble gas budget).

Calibration of cosmogenic noble gas production in ordinary chondrites based on 36 Cl- 36 Ar ages. Part 1: Refined produced rates for cosmogenic 21 Ne and 38 Ar

We measured the concentrations and isotopic compositions of He, Ne, and Ar in bulk samples and metal separates of 14 ordinary chondrite falls with long exposure ages and high metamorphic grades. In addition, we measured concentrations of the cosmogenic radionuclides 10Be, 26Al, and 36Cl in metal separates and in the nonmagnetic fractions of the selected meteorites. Using cosmogenic 36Cl and 36Ar measured in the metal separates, we determined 36Cl-36Ar cosmic-ray exposure (CRE) ages, which are shielding-independent and therefore particularly reliable. Using the cosmogenic noble gases and radionuclides, we are able to decipher the CRE history for the studied objects. Based on the correlation 3He/21Ne versus 22Ne/21Ne, we demonstrate that, among the meteorites studied, only one suffered significant diffusive losses (about 35%). The data confirm that the linear correlation 3He/21Ne versus 22Ne/21Ne breaks down at high shielding. Using 36Cl-36Ar exposure ages and measured noble gas concentrations, we determine 21Ne and 38Ar production rates as a function of 22Ne/21Ne. The new data agree with recent model calculations for the relationship between 21Ne and 38Ar production rates and the 22Ne/21Ne ratio, which does not always provide unique shielding information. Based on the model calculations, we determine a new correlation line for 21Ne and 38Ar production rates as a function of the shielding indicator 22Ne/21Ne for H, L, and LL chondrites with preatmospheric radii less than about 65 cm. We also calculated the 10Be/21Ne and 26Al/21Ne production rate ratios for the investigated samples, which show good agreement with recent model calculations.

A combined vacuum crushing and sieving (CVCS) system designed to determine noble gas paleotemperatures from stalagmite samples

This paper presents a novel extraction device for water and noble gases from speleothem samples for noble gas paleotemperature determination. The “combined vacuum crushing and sieving (CVCS) system” was designed to reduce the atmospheric noble gas contents from air inclusions in speleothem samples by up to 2 orders of magnitude without adsorbing atmospheric noble gases onto the freshly produced grain surfaces, a process that had often hampered noble gas temperature (NGT) determination in the past. We also present the results from first performance tests of the CVCS system processing stalagmite samples grown at a known temperature. This temperature is reliably reproduced by the NGTs derived from Ar, Kr, and Xe extracted from the samples. The CVCS system is, therefore, suitable for routine determinations of accurate NGTs. In combination with stalagmite dating, these NGTs will allow reconstructing past regional temperature evolutions, and also support the interpretation of the often complex stable isotope records preserved in the stalagmites' calcite.

Origin and evolution of reactive and noble gases dissolved in matrix pore water

Reactive and noble gases dissolved in matrix pore water of low permeable crystalline bedrock were successfully extracted and characterized for the fist time based on drillcore samples from the Olkiluoto investigation site (SW Finland). Interaction between matrix pore water and fracture groundwater occurs predominately by diffusion. Changes in the chemical and isotopic composition of gases dissolved in fracture groundwater are transmitted and preserved in the pore water. Absolute concentrations, their ratios and the stable carbon isotope signature of hydrocarbon gases dissolved in pore water give valuable indications about the evolution of these gases in the nearby-flowing fracture groundwaters. Inert noble gases dissolved in matrix pore water and their isotopes combined with their in-situ production and accumulation rates deliver information about the residence time of pore water.