Rare gas isotopic compositions in natural gases of Japan

Isotopic and elemental compositions of rare gases in various types of gas samples collected in the Japanese Islands were investigated. Excess³He was found in most samples. Many samples showed a regionally uniform high³He/⁴He ratio of about 7 times the atmospheric ratio. The He concentrations varied from 0.6 to 1800 ppm, and they were low in CO₂-rich gases and high in N₂-rich gases. Ne isotopic deviations from the atmospheric Ne were detected in most volcanic gases. The deviations and the elemental abundance patterns in volcanic gases can be explained by a mixing between two components, one is mass fractionated rare gases and the other is isotopically atmospheric and is enriched in heavy rare gas elements. Ar was a mixture of mass fractionated Ar, atmospheric Ar and radiogenic Ar, and the contribution of radiogenic⁴⁰Ar was small in all samples. Except for He, elemental abundance patterns were progressively enriched in the heavier rare gases relative to the atmosphere. Several samples were highly enriched in Kr and Xe relative to the abundance pattern of dissolution equilibrium of atmospheric rare gases in water. The component which is highly enriched in heavy rare gases may be released from sedimentary materials in the crust.     

Rare gas isotopes and mass fractionation: An indicator of gas transport into or from a magma

A simple model of mass fractionation may explain the isotopic ratios of rare gases in volcanic materials. Single-stage mass fractionation of atmospheric rare gases predicts an upper limit for²⁰Ne/²²Ne of 10.3 and a lower limit for⁴⁰Ar/³⁶Ar of 280. The rare gas data in volcanic materials seem to support this interpretation.Relatively low⁴⁰Ar/³⁶Ar ratios, as low as 282, have been observed in recent Japanese volcanic rocks. Such a low⁴⁰Ar/³⁶Ar ratio may be explained by mass fractionation of the atmospheric value if the rare gases represent those which were transported into the magma chamber with other volatile elements.Both the amounts and the fractionated rare gas abundance pattern of lighter elements which are observed in pumices from the recent eruption of Mt. Usu, Southern Hokkaido, Japan, suggest the possibility of air injection into its magma chamber. Thus, the fractionation of rare gases in volcanic materials may be a common occurrence, and it must be considered in models for the origin of isotopic differences between rare gases in volcanic materials and the atmosphere.     

He,Ne and Ar isotopic composition of Fe-Mn crusts from the western and central Pacific Ocean and implications for their genesis

The noble gas nuclide abundances and isotopic ratios of the upmost layer of Fe-Mn crusts from the western and central Pacific Ocean have been determined. The results indicate that the He and Ar nu- clide abundances and isotopic ratios can be classified into two types: low 3He/4He type and high 3He/4He type. The low 3He/4He type is characterized by high 4He abundances of 191×10-9 cm3·STP·g-1 on average, with variable 4He, 20Ne and 40Ar abundances in the range (42.8―421)×10-9 cm3·STP·g-1, (5.40―141)×10-9 cm3·STP·g-1, and (773―10976)×10-9 cm3·STP·g-1, respectively. The high 3He/4He samples are characterized by low 4He abundances of 11.7×10-9 cm3·STP·g-1 on average, with 4He, 20Ne and 40Ar abundances in the range of (7.57―17.4)×10-9 cm3·STP·g-1, (10.4―25.5)×10-9 cm3·STP·g-1 and (5354―9050)×10-9 cm3·STP·g-1, respectively. The low 3He/4He samples have 3He/4He ratios (with R/RA ratios of 2.04―2.92) which are lower than those of MORB (R/RA=8±1) and 40Ar/36Ar ratios (447―543) which are higher than those of air (295.5). The high 3He/4He samples have 3He/4He ratios (with R/RA ratios of 10.4―12.0) slightly higher than those of MORB (R/RA=8±1) and 40Ar/36Ar ratios (293―299) very similar to those of air (295.5). The Ne isotopic ratios (20Ne/22Ne and 21Ne/22Ne ratios of 10.3―10.9 and 0.02774―0.03039, respectively) and the 38Ar/36Ar ratios (0.1886―0.1963) have narrow ranges which are very similar to those of air (the 20Ne/22Ne, 21Ne/22Ne, 38Ar/36Ar ratios of 9.80, 0.029 and 0.187, respectively), and cannot be differentiated into different groups. The noble gas nuclide abundances and isotopic ratios, together with their regional variability, suggest that the noble gases in the Fe-Mn crusts originate primarily from the lower mantle. The low 3He/4He type and high 3He/4He type samples have noble gas characteristics similar to those of HIMU (High U/Pb Mantle)- and EM (Enriched Mantle)-type mantle material, respectively. The low 3He/4He type samples with HIMU-type noble gas isotopic ratios occur in the Magellan Seamounts, Marcus-Wake Seamounts, Marshall Island Chain and the Mid-Pacific Sea- mounts whereas the high 3He/4He type samples with EM-type noble gas isotopic ratios occur in the Line Island Chain. This difference in noble gas characteristics of these crust types implies that the MagellanSeamounts, Marcus-Wake Seamounts, Marshall Is- land Chain, and the Mid-Pacific Seamounts originated from HIMU-type lower mantle material whereas the Line Island Chain originated from EM-type lower mantle material. This finding is consistent with varia- tions in the Pb-isotope and trace element signatures in the seamount lavas. Differences in the mantlesource may therefore be responsible for variations in the noble gas abundances and isotopic ratios in the Fe-Mn crusts. Mantle degassing appears to be the principal factor controlling noble gas isotopic abundances in Fe-Mn crusts. Decay of radioactive isotopes has a negligible influence on the nuclide abundances and isotopic ratios of noble gases in these crusts on the timescale of their formation.     

Noble gases in submarine pillow volcanic glasses

Fifteen submarine glasses from the East Pacific Rise (CYAMEX), the Kyushu-Palau Ridge (DSDP Leg 59) and the Nauru Basin (DSDP Leg 61) were analysed for noble gas contents and isotopic ratios. Both the East Pacific Rise and Kyushu-Palau Ridge samples showed Ne excess relative to Ar and a monotonic decrease from Xe to Ar when compared with air noble gas abundance. This characteristic noble gas abundance pattern (type 2, classified by Ozima and Alexander) is interpreted to be due to a two-stage degassing from a noble gas reservoir with originally atmospheric abundance. In the Kyushu-Palau Ridge sample, noble gases are nearly ten times more abundant than in the East Pacific Rise samples. This may be attributed to an oceanic crust contamination in the former mantle source.There is no correlation between the He content and that of the other noble gas in the CYAMEX samples. This suggests that He was derived from a larger region, independent from the other noble gases.Except where radiogenic isotopes are involved, all other noble gas isotopic ratios were indistinguishable from air noble gas isotopic ratios. The³He/⁴He in the East Pacific Rise shows a remarkably uniform ratio of (1.21±0.07)×10^?5, while the⁴⁰Ar/³⁶Ar ranges from 700 to 5600.     

Thermal release characteristics of spallogenic He,Ne, and Ar from the Carbo iron meteorite

The thermal release patterns of He, Ne and Ar from samples of the Carbo iron meteorite show that virtually no fractionation of³He,⁴He,²¹Ne and³⁸Ar occurs. Thus, conclusions about iron meteorites based on measured noble gas ratios will be unaffected by gas loss, and measurement of these ratios cannot yield information about possible loss. Further, noble gas loss cannot explain the abnormal elemental and isotopic patterns observed in some iron meteorites, notably hexahedrites.     

A Portable Membrane Contactor Sampler for Analysis of Noble Gases in Groundwater

To enable a wider use of dissolved noble gas concentrations and isotope ratios in groundwater studies, we have developed an efficient and portable sampling device using a commercially available membrane contactor. The device separates dissolved gases from a stream of water and collects them in a small copper tube (6 mm in diameter and 100 mm in length with two pinch‐off clamps) for noble gas analysis by mass spectrometry. We have examined the performance of the sampler using a tank of homogeneous water prepared in the laboratory and by field testing. We find that our sampling device can extract heavier noble gases (Ar, Kr, and Xe) more efficiently than the lighter ones (He and Ne). An extraction time of about 60 min at a flow rate of 3 L/min is sufficient for all noble gases extracted in the sampler to attain equilibrium with the dissolved phase. The extracted gas sample did not indicate fractionation of helium (³He/⁴He) isotopes or other noble gas isotopes. Field performance of the sampling device was tested using a groundwater well in Vienna and results were in excellent agreement with those obtained from the conventional copper tube sampling method.     

Atmospheric noble gases in volcanic glasses from the southern Lau Basin: origin from the subducting slab?

Noble gas concentrations and isotopic compositions have been determined for four submarine volcanic glasses from the Valu Fa Ridge (VFR) in the southern Lau Basin. The samples are the least differentiated ones from this area, and they display enrichments in fluid-mobile elements similar to the nearby island arc. ³He/⁴He ratios are slightly below average MORB (6.8–7.8 times atmospheric), whereas Ne, Ar, Kr, and Xe have isotopic compositions very similar to air. Together with previously published data from the Valu Fa Ridge and other spreading segments in the Lau Basin, our data show a systematic latitudinal variation of increasing Ne, Ar, Kr, and Xe abundances from north to south as well as Ne and Ar isotopic compositions changing from MORB-like to atmosphere-like in the same direction. Moreover, isotopic compositions and noble gas abundances of the lavas correlate strongly with Ba/Nb ratios and H₂O concentrations. Based on these observations and mass balance arguments, we propose that the atmospheric noble gases come from the subducting oceanic crust and are not due to shallow contamination with air dissolved in seawater or assimilation of old crust. Our data suggest that the noble gases released from the subducting slab are atmospheric and thus contain little or no solar He and Ne. In addition to the fact that ratios of He to heavy noble gases are small in aged ocean crust, He has possibly fractionated from the other noble gases due to its higher diffusivity, and thus He transport from the subducting slab into the mantle wedge is probably insignificant. We propose that the ³He/⁴He ratios lower than MORB observed in the VFR lavas result from radiogenic ingrowth of He in a highly depleted, and hence degassed, mantle wedge after the enrichment of U and Th released from the downgoing slab.     

Noble gases in a section across the vapor dominated geothermal field of Larderello,Italy

Noble gases were studied in six wells, located on a 4.5 km south to north section across the Larderello field. Depth of wells, flow and gas/steam ratios are known to increase from south to north. Exploitation progressed in the same direction. The following noble gas patterns are observable: (a) Atmospheric Ar, Kr and Xe reflect productions of gas-depleted water at Colombaia 2 and progressively more gas-enriched steam towards the Gabbro wells. (b) Radiogenic⁴He and⁴⁰Ar are observed in increasing concentrations from south to north. (c) The radiogenic and atmospheric gases reveal a positive correlation, indicating that the recharging water enters deep into the system, and gets well mixed with the radiogenic gases prior to the steam separation. (d) Gas contents and relative abundances of radiogenic argon decrease with production, thus supplying markers for the degree of exploitation in a well and a guide for optimum well spacing. (e) Excess neon over argon is observed and discussed in terms of crustal origin versus possible fractionation of atmospheric noble gases due to pertial steam separation.     

Inert gases in twelve particles and one “dust” sample from Luna 16

The inert gases were measured mass-spectrometrically in 12 fragments and 1 “dust” sample from Luna 16. The fragments were classified petrologically by microscopic inspection. The major petrologic types were breccias and basalts. The former were much richer in trapped gases than the latter, and were apparently formed by the welding of local fines. However, there was no clear-cut difference in gas content of either breccias or basalts between zone A (top) and zone G (bottom). The⁴He/²⁰Ne ratio of the breccias (average 49) was systematically smaller than that of the basalts (average 78), probably because of He-Ne fractionation during or after the formation of the breccias. We suggest that the⁴He/²⁰Ne ratios of bulk fines in general may reflect the proportions of basaltic and breccia (plus cindery glasses) fragments in the fines. Substantial variations of⁴He/³He were found, which could not be explained with the presence of variable proportions of cosmogenic³He_c. Either the solar-wind value has changed in time, or the fragments with the small ratios were exposed to solar flares rich in³He and/or⁴He. Exposure ages of four fragments are several hundred million years. The⁴⁰Ar/³⁶Ar slopes of breccias and basalts are identical: 0.65.     

The origin of josephinites: a new noble gas study

We performed a complete noble gas study on eight different josephinites and one oregonite. The ⁴He/³He ratios range between 100,000 and 330,000 and are probably due to a combination of a MORB He-component from the Josephinite Peridotite massif, where these nickel-iron specimens are found, and either atmospheric He or radiogenic He from the underlying continental or subcontinental basement. The ⁴⁰Ar/³⁶Ar ratios of 302 to 381 are slightly higher than the ratio of air-argon. The neon, krypton and xenon isotopic ratios are identical to the corresponding air ratios. We cannot confirm large³He and²¹Ne excesses published earlier. The observed noble gas isotopic signatures are in agreement with a formation of josephinites near the surface. The data do not favour a deep mantle origin or a formation at the mantle-core boundary as proposed before.     

Rare gases in a phlogopite nodule and a phlogopite-bearing peridotite in South African kimberlites

Rare gas isotopes in a phlogopite nodule and a phlogopite-bearing peridotite nodule in South African kimberlites were studied to examine the state of rare gases in the deep interior of the kimberlite region.Within the experimental error of 1 ～ 2%, rare gas isotopic compositions are atmospheric except for radiogenic⁴He and⁴⁰Ar. No excess¹²⁹Xe was observed.In phlogopite, Ne is more depleted, whereas the heavier rare gases are more enriched than the atmospheric rare gases relative to³⁶Ar.Together with other data these results suggest that the state of rare gases in the upper mantle of the South African kimberlite region might have been changed from the typical primitive mantle by a process such as mixing of crustal materials.     

Mid-ocean ridge popping rocks: implications for degassing at ridge crests

The vesicle size distribution (VSD) and rare gas abundances in popping rocks from 14°N on the Mid-Atlantic Ridge provide constraints on the behavior of volatiles during ridge crest volcanism. These popping rocks, which contain 16–18 volume percent vesicles, are rare mid-ocean ridge basalt (MORB) magmas which appear to have retained much of their volatile inventory. The logarithm of vesicle population density displays the same linear correlation with decreasing size in two of the samples studied. This implies that continuous and simultaneous nucleation and bubble growth have occurred during magma ascent, with no significant perturbations due to accumulation, coalescence or loss of bubbles. In contrast, most MORB magmas display low vesicularities and we suggest that they have suffered some degree of pre-eruptive vesicle loss. We tentatively propose that large vesicles are produced by coalescence when MORB melt is at rest in chambers and conduits, and may be lost during early gas-rich episodes. Most MORB would represent residual liquids which erupt after vesicle loss has occurred, whereas popping rocks would represent a rare case where physical sorting of vesicles from melt did not occur, because storage in a magma chamber did not occur.The rare gas concentrations in the studied popping rocks are the highest yet measured in glassy ridge basalts ([He] > 50 μccSTP/g). The rare gas abundance pattern of these popping rocks probably resembles the pattern for non-vesiculated MORB magma and potentially reflects that of the depleted mantle source. This pattern is similar to the “mean MORB” pattern (computed from MORB glasses with⁴⁰Ar/³⁶Ar > 10,000) although a higher enrichment in He (and possibly Ne) compared to the heavier rare gases is observed in MORB. The overall similarity in abundance patterns for MORB and popping rocks indicates that vesiculation and vesicle loss do not fractionate the ArKrXe relative abundances from those in non-vesiculated magma, and that the modern flux ratios of these gases at ridges are similar to their elemental ratios in the depleted mantle. The degassing flux of He at ridge crests estimated from the MORB He deficit relative to popping rocks is comparable to the flux derived from the³He budget for the abyssal ocean. This suggests that degassing at ridges may be strongly influenced by the dynamics and style of submarine volcanism.     

Rare gases,water, and carbon in kaersutites

Kaersutites from Kakanui, New Zealand and from three localities in the southwestern United States have been analyzed for rare gases, water and carbon to investigate the volatile signature of the sub-continental mantle. This study does not confirm the high ³He/⁴He and ²¹Ne/²²Ne ratios reported by Saito et al. [1] for the Kakanui kaersutite. Instead, a ³He/⁴He ratio of 6 R_A and atmospheric ²¹Ne/²²Ne ratios were measured which are consistent with our current knowledge of the earth's mantle. A low ⁴⁰Ar/³⁶Ar of 320 and more than 10^?8 cm³/g of ³⁶Ar confirms the argon results of Saito et al. and indicates that significant quantities of ³⁶Ar reside in this portion of the mantle. Kaersutites from the southwestern United States (Arizona) have a heterogeneous helium isotope signature, ranging from 8.8 R_A at San Carlos to 0.46 at Hoover Dam. All D/H ratios for the water in kaersutites (?56‰ to ?78‰) represent typical mantle values with no apparent correlation with ³He/⁴He. The correlation of increasing carbon content (140–400 ppm) with increasing δ¹³C (?24.5‰ to ?16.7‰) may reflect differences in the proportions of oxidized and reduced carbon in these samples.     

Water-saturated oceanic lavas from the Manus Basin: volatile behaviour during assimilation–fractional crystallisation–degassing (AFCD)

We have analysed volatiles (H₂O, He, Ar, CO₂) in differentiated (basaltic andesite, dacite) volcanic glasses dredged at a depth of ca. 2000 m in the eastern part of the Manus Basin between 151°20′ and 152°10′ E. These samples have Sr–O–B isotopic ratios that show that they most likely represent lavas evolved from a common magma source. Since these glasses are very fresh, they provide a unique opportunity to study the behaviour of magmatic volatiles during assimilation–fractional crystallisation–degassing (AFCD). The samples are highly vesicular (up to 18%) and the volatiles trapped in vesicles consist predominantly of H₂O with minor amounts of CO₂, and the concentration of water in the glasses indicates that H₂O saturation was attained. Rare gases except helium are atmospheric in origin, and the ³He/⁴He ratios and the CO₂/³He ratios are respectively lower and higher than those typical of Mid-Ocean Ridge Basalt (MORB), and appear to correlate with the degree of differentiation. AFCD allows efficient degassing of mantle-derived volatiles and contribution of crust-derived and atmosphere-derived volatiles. Given the widespread occurrence of differentiated magmatism at arcs, we suggest that AFCD is responsible for large-scale occurrence of ³He-rich crustal fluids and of atmospheric-like rare gases in arc emanations, and that most of the volatiles are lost continuously during fractional crystallisation, rather than catastrophically during eruptions.     

Trapped solar and cosmogenic noble gas abundances in Apollo 15 and 16 deep drill samples

Abundances and isotopic compositions of all the stable noble gases have been measured in 19 different depths of the Apollo 15 deep drill core, 7 different depths of the Apollo 16 deep drill core, and in several surface fines and breccias. All samples analyzed from both drill cores contain large concentrations of solar wind implanted gases, which demonstrates that even the deepest layers of both cores have experienced a lunar surface history. For the Apollo 15 core samples, trapped⁴He concentrations are constant to within a factor of two; elemental ratios show even greater similarities with mean values of⁴He/²²Ne= 683±44,²²Ne/³⁶Ar= 0.439±0.057,³⁶Ar/⁸⁴Kr= 1.60±0.11·10³, and⁸⁴Kr/¹³²Xe= 5.92±0.74. Apollo 16 core samples show distinctly lower⁴He contents,⁴He/²²Ne(567±74), and²²Ne/³⁶Ar(0.229±0.024), but their heavy-element ratios are essentially identical to Apollo 15 core samples. Apollo 16 surface fines also show lower values of⁴He/²²Ne and²²Ne/³⁶Ar. This phenomenon is attributed to greater fractionation during gas loss because of the higher plagioclase contents of Apollo 16 fines. Of these four elemental ratios as measured in both cores, only the²²Ne/³⁶Ar for the Apollo 15 core shows an apparent depth dependance. No unambiguous evidence was seen in these core materials of appreciable variations in the composition of the solar wind. Calculated concentrations of cosmic ray-produced²¹Ne,⁸⁰Kr, and¹²⁶Xe for the Apollo 15 core showed nearly flat (within a factor of two) depth profiles, but with smaller random concentration variations over depths of a few cm. These data are not consistent with a short-term core accretion model from non-irradiated regolith. The Apollo 15 core data are consistent with a combined accretion plus static time of a few hundred million years, and also indicate variable pre-accretion irradiation of core material. The lack of large variations in solar wind gas contents across core layers is also consistent with appreciable pre-accretion irradiation. Depth profiles of cosmogenic gases in the Apollo 16 core show considerably larger concentrations of cosmogenic gases below ～65 cm depth than above. This pattern may be interpreted either as an accretionary process, or by a more recent deposition of regolith to the upper ～70 cm of the core. Cosmogenic gas concentrations of several Apollo 16 fines and breccias are consistent with ages of North Ray Crater and South Ray Crater of ～50·10⁶ and ～2·10⁶ yr, respectively.     

N<Subscript>2</Subscript>, Ar,and He as a tool for discriminating sources of volcanic fluids with application to Vulcano,Italy

A detailed analysis of published data on the N₂, Ar, and He content and Ar and He isotopic composition of fumarolic fluids from Vulcano crater (south Italy) supports a model with two endmembers comprising magmatic and hydrothermal fluids with correspondingly low and high H₂O content. The magmatic component with the highest ³He/⁴He and highest absolute concentrations of N₂, Ar, and He also has the lowest N₂/Ar and N₂/He ratios (∼300 and ∼500, respectively). In contrast, the hydrothermal endmember, with the lower ³He/⁴He and lower absolute N₂, Ar, and He abundances, has high N₂/Ar (∼1,000) and high N₂/He (>3,000) ratios. The hydrothermal component is also characterized by the highest ⁴⁰Ar/³⁶Ar ratios (>1,000) and is proposed to be the main carrier of metamorphic gases from the arc crust.     

Planetary-type rare gases in an upper mantle-derived amphibole

All twenty-three stable rare gas isotopes have been measured in a mantle-derived amphibole, kaersutite. The elemental abundance pattern of the rare gases is similar to the “planetary” rare gas pattern as defined by carbonaceous chondrites. The³He/⁴He ratio, (4.9 ± 0.6) × 10^?5, is suggestive of primordial He degassing from the mantle. Excess²¹Ne is present. The measured⁴⁰Ar/³⁶Ar ratio,400 ± 5, may represent a mantle⁴⁰Ar/³⁶Ar ratio <240 when corrected for radiogenic⁴⁰Ar. The heavy isotopes of Kr and t0he Xe isotopes are within error of the atmosphere values.     

Primordial gases in graphite-diamond-kamacite inclusions from the Haveröureilite

Stepwise heating experiments on separated graphite-diamond-kamacite aggregates have revealed a pronounced difference in the release patterns of spallogenic³He and trapped gases. About half the³He is released at T ? 920°C, without being accompanied by significant amounts of primordial gases; the latter, together with the remaining³He, is given off only at T ? 1200°C. Acid treatment of an aliquant dissolved about 2/3 of the total Fe in the sample but did not cause a significant change in the gas concentrations. It is concluded that (a) there is no evidence for a loss of spallogenic³He from the graphite-diamond-kamacite aggregates, (b) one major constituent of the aggregates - graphite - is almost void of trapped gases, (c) kamacite is not a main carrier of the gases. This leaves diamond as the most probable site of the primordial gases.The elemental abundance pattern in the noble gases is essentially as reported previously. In particular, the excellent correlation between relative depletion factors, normalized to the cosmic abundance ratios, and the respective ionisation energies is confirmed. Other important features of the trapped gases are a²⁰Ne/²²Ne ratio of 12.3 ± 0.6, intermediate between solar wind and solar flare implanted Ne,³⁶Ar/³⁸Ar = 5.20 ± 0.06 and a measured⁴⁰Ar/³⁶Ar ratio (before blank correction) of 0.0076.Possible modes of trapping of the noble gases are discussed.     

Factors controlling the noble gas abundance patterns of deep-sea basalts

A number of processes may modify the noble gas composition of silicate liquids so that the composition of noble gases observed in glassy margins of deep-sea basalts is not that of the upper mantle. Differential solubility enhances the light noble gases relative to the heavier gases; however, we demonstrate that the observed abundance pattern cannot be attributed to solubility of noble gases with atmospheric proportions. Partial melting and fractional crystallization increase the noble gas content of all species relative to mantle concentrations, but do not fractionate their relative abundances. Noble gases may be lost from an ascending magma in various ways, the most important, however, may be exclusion of gas from crystals forming at the time of solidification, which is shown to result in marked loss of gas from the basalt. Small amounts of low-temperature alteration of solidified basalt can produce dramatic changes in the noble gas abundance pattern, since the adsorption coefficients for the different noble gas favor uptake of heavy species relative to the light species. Atmospheric contamination can account for observed variations in the ⁴⁰Ar/³⁶Ar ratio of oceanic basalts. The degree of crystallinity of glassy margins of deep-sea basalts may control the helium abundance of these samples; however, the uniform ³He/⁴He values reported apparently reflect a relatively constant proportion of radiogenic and primordial helium in the mantle.     

Atmospheric noble gas signatures in deep Michigan Basin brines as indicators of a past thermal event

Atmospheric noble gases (e.g., ²²Ne, ³⁶Ar, ⁸⁴Kr, ¹³⁰Xe) in crustal fluids are only sensitive to subsurface physical processes. In particular, depletion of atmospheric noble gases in groundwater due to boiling and steam separation is indicative of the occurrence of a thermal event and can thus be used to trace the thermal history of stable tectonic regions. We present noble gas concentrations of 38 deep brines (~ 0.5–3.6 km) from the Michigan Basin. The atmospheric noble gas component shows a strong depletion pattern with respect to air saturated water. Depletion of lighter gases (²²Ne and ³⁶Ar) is stronger compared to the heavier ones (⁸⁴Kr and ¹³⁰Xe). To understand the mechanisms responsible for this overall atmospheric noble gas depletion, phase interaction models were tested. We show that this atmospheric noble gas depletion pattern is best explained by a model involving subsurface boiling and steam separation, and thus, consistent with the occurrence of a past thermal event of mantle origin as previously indicated by both high ⁴He/heat flux ratios and the presence of primordial mantle He and Ne signatures in the basin. Such a conceptual model is also consistent with the presence of past elevated temperatures in the Michigan Basin (e.g., ~ 80–260 °C) at shallow depths as suggested by previous thermal studies in the basin. We suggest that recent reactivation of the ancient mid-continent rift system underneath the Michigan Basin is likely responsible for the release of both heat and mantle noble gases into the basin via deep-seated faults and fracture zones. Relative enrichment of atmospheric Kr and Xe with respect to Ar is also observed, and is interpreted as reflecting the addition of sedimentary Kr and Xe from associated hydrocarbons, following the hydrothermal event. This study pioneers the use of atmospheric noble gases in subsurface fluids to trace the thermal history of stable tectonic regions.