高分辨电感耦合等离子体质谱法测定铀矿石样品中234U/238U、230Th/232Th和228Ra/226Ra同位素比值 

采用氢氟酸-硝酸-盐酸混合酸密闭消解含铀矿石样品,用阴离子交换树脂、阳离子交换树脂和锶特效树脂逐级分离富集铀、钍和镭。使用高分辨电感耦合等离子体质谱(HR-ICPMS)测定分离纯化液中234U/238U2、30Th/232Th和228Ra/226Ra同位素。比值的测量精密度取决于比值的大小和对应核素浓度的大小。对质量浓度为10 ng/mL天然铀测量液,234U/238U的测量精密度优于1.2%;对230Th质量浓度为0.6ng/mL且230Th和232Th质量浓度接近的测量液,230Th/232Th的测量精密度为1.2%;对228Ra质量浓度为0.48 pg/mL且228Ra和226Ra质量浓度接近的测量液,228Ra/226Ra的测量精密度为4.0%。     

平面型高纯锗低能γ谱仪测定铀矿样中^235U,^238U,^226Ra及^232Th含量

本文对选用低能γ射线测定铀矿中的~(235)U、~(238)U、~(226)Ra、~(232)Th含量进行了讨论,提出了一种对样品进行自吸收校正的简单准确方法,对铀矿样中的~(235)U、~(238)U、或~(235)U/~(238)U比值测定获得了较高的分析精度和准确度。     

一次分解试样测定地质样品中~(230)Th,~(232)Th和~(234)U/~(238)U,~(230)Th/~(232)Th

试验了用~(234)Th示踪,一次分解试样测定~(234)Th,~(232)Th和~(234)U/~(238)U,~(230)Th/~(232)Th的快速方法。试样经Na_2O_2熔融分解,并以P350萃取色层法分离铀、钍。然后分别电沉积制备无自吸收铀、钍α源进行α谱测量。本法适用于铀矿石、岩石和土壤试样的测定。     

南京直立人的U/Th和U/Pa年代

中国直立人化石的准确定年对于研究人类演化有着极为重要的意义。1993～1994年在南京汤山葫芦洞发现的两个直立人头盖骨化石和一枚牙化石被称为“南京直立人”。其中1号头盖骨化石之上的方解石钙板的U/Th年龄为53.3_(-1.2)~(+1.5)万年;但考虑到定年的准确性,则为53.3_(-3.0)~(+3.5)万年。其~(231)Pa/~(235)U活度比值为0.998±0.006。这表明“南京直立人”的年代应该大于50万年。与”南京直立人”伴生的动物牙化石U/Th年代为18.5～29.0万年;U/Pa年代为13.7～17.2万年。此外,对于同一颗牙化石,牙釉的年龄小于牙本质的年龄。同一样品的U/Pa年龄也显著小于其U/Th年龄。因此,牙化石的U摄取过程并不符合U早期摄取模式。多数牙化石分析点在~(234)U/~(238)U-~(230)Th/~(238)U图上落在位于U早期摄取和线性摄取模式曲线之间,指示牙化石的U摄取过程很可能介于上述两种模式之间。如果这一假设成立,那么牙化石的U/Th和U/Pa线性摄取模式年龄则为其年代的上限。因为不受U摄取过程~(234)U/~(238)U变化的影响,U/Pa线性摄取模式年龄比U/Th较为可靠。最小的U/Pa线性摄取模式年龄为1Ma,这是”南京直立人”上限年龄的估计。从定年结果看,”南京直立人”可能生活在海洋同位素(MIS)16阶段,但这不是最终结论。     

离子交换纤维法的新应用

天然水中~(234)U/~(238)U、~(230)Th/~(232)Th和~(226)Ra/~(228)Ra放射性同位素比值,已做为水文地球化学研究和水化找矿的重要参数。 IEF——离子交换纤维是新型功能高分子材料,适用于大容量高效富集、分离和净化。经研究,用IEF可以现场富集天然水中的U、Th和Ra元素,我们设计了IEF法野外现场     

环境水样中铀、钍、镭和铅同位素及其比值的系统分析

本文研究了从5L水中用铁、铅、钡和铈作载体,系统分析~(234)U、~(238)U、~(228)Th、~(230)Th~(232)Th、~(224)Ra、~(226)Ra、~(228)Ra和~(210)Pb的含量或比值。铀、钍经Fe(OH)_3沉淀富集后用TBP萃淋树脂柱分离,用激光荧光和比色法测定,同位素比值用α谱仪测量,化学回收率在90％以上,测量下限分别为1μg/L和3μg/L。镭、铅经硫酸盐沉淀富集后,用EDTA在不同pH条件下分离,~(224)Ra和~(226)Ra用射气法测定,~(228)Ra和~(210)Pb分别用其β子体~(228)Ac和~(210)Bi在低本底β装置上测量,测量下限分别为2.5×10~(-2)、8×10~(-3)、4×10~(-3)和5×10~(-3)Bq/L。     

THE APPLICATION OF INDUCTIVELY COUPLED PLASMA-QUADRUPOLE MASS SPECTROMETRY TO FOSSIL TEETH FOR U-TH ISOTOPE ANALYSIS

四极杆电感耦合等离子体质谱仪(Inductively Coupled Plasma-Quadrupole Mass Spectrometry,简称ICP-QMS)可用于U和Th同位素分析.目前,ICP-QMS能实现精度大约为0.3％(U)和1％(Th)的测量分析,可提供误差在1％～10％的230Th/U年代数据.本文用ICP-QMS分析了采自意大利南都Loreto旧石器地点的4颗马牙化石样品,并对已发表的UTEVA树脂提纯U和Th的流程做了进一步改进,使其适用于动物牙化石样品.样品中的U和Th含量的平均测量精度(2σ)分别为0.3％和0.6％;234U/235U和230Th/238U活度比平均精度(2σ)分别为0.3％和0.8％.数据表明同一颗牙化石的不同组织的U含量可有数量级差别,同时它们的U -Th同位素活度比也可显著地离散(＞2σ),从而导致不一致的230Th/U年代结果.如今测定的各牙组织的U-Th同位素数据可用于模拟U的迁移历史;U-系分析与电子自旋共振测年技术相结合或可更好地估计样品的地质年代.     

洞穴碳酸盐230Th-234U-238U测年初始钍校正的等时线研究

初始钍的校正是不纯沉积碳酸盐230Th 234U 238U测年的一个重要方面，洞穴石笋初始Th校正通常采用230Th/232Th的原子比值为（4.4±2.2）×10-6。多年来4种不同的等时线方法应用到不纯碳酸盐测年初始Th的校正中，其中全样品的等时线方法是目前公认的较为完善的一种方法。通过测定云南同一石笋2个不同层位的9个样品的U、Th同位素组成,并进行等时线分析，结果表明2层样品初始钍230Th/232Th原子比值分别为（3.5±2.8）×10-6和（10.6±2.2）×10-6，这说明即使在同一地区，由于其混入Th来源的复杂性，230Th/232Th初始比值在同一样品不同层位仍可能有较大的差异，因此不能够完全采用单一层位等时线获得的初始值对整个样品进行校正。考虑到在实验测量过程中，232Th含量的过高对于230Th的准确测定也有很大的影响，应尽量选择纯净石笋样品进行测年研究，在样品的选择和前处理过程中就减少初始钍的影响，这对获得高精度的测年结果有着重要的意义。     

234U/238U法测定石笋年龄

<正> 应用230Th/234U法研究洞穴沉积物年代已取得可靠结果,成功的为距今35万年以来的洞穴沉积物标上时标。近十几年来,为了开展老于35万年洞穴沉积物年代学研究,曾探讨应用234U/238U法和ESR法研究碳酸钙沉积物年代。目前已在234U/238U法研究洞穴沉积物年代方面取得成果。然而,由于样品条件不适合,洞穴采样困难以及样品初始234U/238U放射性比值确定存在问题和争论,这方面的研究尚待进一步深入。本文报道一个石笋五个不同生长层样品的234U/238U年代测定结果。试图对老于35万年的洞穴沉积物年龄研究,提供一个可用方法。并对相应时期的古气候环境进行探讨。      

文石-方解石石笋U/Th体系的封闭性判断及意义

湖南省龙山县莲花洞两根大型石笋LLl(文石-方解石型)和LL5(文石型)ICP-MS230Th结果表明,82个年龄数据并不完全符合石笋生长层序律.根据U/Th同位素比值、沉积和矿物学特征,分析了同位素体系开放度对建立石笋正确年代学模式的影响.莲花洞LLl石笋全新世以来234U/238U对230Th/238U的比值具有谐和性特征并且230Th年龄层序正常,说明文石矿物基本接近U/Th同位素封闭系统,实测年龄基本可靠.10～40 ka期间234U/238U与230Th/238U离散度较大和矿物具有溶蚀、风化现象,表明体系发生U加入/流失作用.LL5石笋60～80 ka期间封闭性较好,实测年龄可信.上述结果表明,同一洞穴中文石石笋U/Th同位素体系开放度与时间的关系并不是线性关系,沉积时水文和物理化学性质以及随后的保存状况是决定洞穴文石石笋同位素封闭性的关键因素.     

Factors controlling the groundwater transport of U, Th, Ra, and Rn

A model for the groundwater transport of naturally occurring U, Th, Ra, and Rn nuclides in the²³⁸U and²³²Th decay series is discussed. The model developed here takes into account transport by advection and the physico-chemical processes of weathering, decay, α-recoil, and sorption at the water-rock interface. It describes the evolution along a flowline of the activities of the²³⁸U and²³²Th decay series nuclides in groundwater. Simple sets of relationships governing the activities of the various species in solution are derived, and these can be used both to calculate effective retardation factors and to interpret groundwater data. For the activities of each nuclide, a general solution to the transport equation has been obtained, which shows that the activities reach a constant value after a distance ϰ_i, characteristic of each nuclide. Where ϰ_i is much longer than the aquifer length, (for²³⁸U,²³⁴U, and²³²Th), the activities grow linearly with distance. Where gKⁱ is short compared to the aquifer length, (for²³⁴Th,²³⁰Th,²²⁸Th,²²⁸Ra, and²²⁴Ra), the activities rapidly reach a constant or quasi-constant activity value. For²²⁶Ra and²²²Rn, the limiting activity is reached after 1 km. High δ²³⁴U values (proportional to the ratio^ɛ234Th/^W238U) can be obtained through high recoil fraction and/or low weathering rates. The activity ratios²³⁰Th/²³²Th,²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra have been considered in the cases where either weathering or recoil is the predominant process of input from the mineral grain. Typical values for weathering rates and recoil fractions for a sandy aquifer indicate that recoil is the dominant process for Th isotopic ratios in the water. Measured data for Ra isotope activity ratios indicate that recoil is the process generally controlling the Ra isotopic composition in water. Higher isotopic ratios can be explained by different desorption kinetics of Ra. However, the model does not provide an explanation for²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra activity ratios less than unity. From the model, the highest²²²Rn emanation equals 2ɛ. This is in agreement with the hypothesis that²²²Rn activity can be used as a first approximation for input by recoil (Krishnaswamiet al 1982). However, high²²²Rn emanation cannot be explained by production from the surface layer as formulated in the model. Other possibilities involve models including surface precipitation, where the surface layer is not in steady-state.     

Precise two chronometer dating of Pleistocene travertine: The Th/U and Raex/Ra(0) approach

In order to determine the geochemical evolution of a freshwater limestone cave system located in central Switzerland (Hell Grottoes at Baar/Zug,) young postglacial tufaceous limestone and travertine precipitates were investigated using the ²³⁰Th/²³⁴U ingrowth system. Additional analyses of further radionuclides within the ²³⁸U decay chain, i.e. ²²⁶Ra and ²¹⁰Pb, showed that the Th/U chronometer started with insignificant inherited ²³⁰Th over the entire formation period of the travertine setting (i.e. ²³⁰Th(0)=0). A contribution from detrital impurities with ²³⁰Th/²³⁴U in secular equilibrium could be precisely subtracted by applying isochron dating of cogenetic phases and recently formed travertine. The resulting precise ²³⁰Th/²³⁴U formation ages were found to be consistent with the geological stratigraphy and were furthermore used to demonstrate the applicability of the next geologically important chronometer in the ²³⁸U-decay series, based on decay of excess ²²⁶Ra normalized to the initial, i.e.²²⁶Ra_ex/²²⁶Ra(0). This system is suitable for dating phases younger than 7000 yr when the correction of a detritus component increasingly limits the precision of the ²³⁰Th/²³⁴U chronometer. Analytical solutions of the coupled ²³⁴U/²³⁰Th/²²⁶Ra radionuclide system predicted that the ²²⁶Ra_ex/²²⁶Ra(0) chronometer is independent of the actual ²³⁰Th activity build up from decay of ²³⁴U, if the systems starts with zero inherited ²³⁰Th(0). The data set confirmed this hypothesis and showed furthermore that the initially incorporated ²²⁶Ra excess must have remained almost uniform in all limestone over a period of at least 7000 yr, i.e. 4–5 half-lives of ²²⁶Ra. This is concluded because (i) the ²²⁶Ra_ex/²²⁶Ra(0) ages agreed well with those derived from ²³⁰Th/²³⁴U, (ii) all data plot within uncertainty on the ²²⁶Ra_ex/²²⁶Ra(0) decay curve and (iii) the atomic Ba/Ca ratio was found to be constant in the travertine material independent of the sample ages. Provided that such boundary conditions hold, ²²⁶Ra_ex/²²⁶Ra(0) should be applicable to materials which are suitable for ²³⁰Th/²³⁴U dating in sedimentology and oceanography, i.e. travertine, corals, phosphorites, etc., and should strongly support ²³⁰Th/²³⁴U for samples that have been formed a few thousand years ago.     

Th/U/U and Pa/U ages from a single fossil coral fragment by multi-collector magnetic-sector inductively coupled plasma mass spectrometry

The ²³⁰Th/²³⁴U/²³⁸U age dating of corals via alpha counting or mass spectrometry has significantly contributed to our understanding of sea level, radiocarbon calibration, rates of ocean and climate change, and timing of El Nino, among many applications. Age dating of corals by mass spectrometry is remarkably precise, but many samples exposed to freshwater yield inaccurate ages. The first indication of open-system ²³⁰Th/²³⁴U/²³⁸U ages is elevated ²³⁴U/²³⁸U_initial values, very common in samples older than 100,000 yr. For samples younger than 100,000 yr that have ²³⁴U/²³⁸U_initial values close to seawater, there is a need for age validation. Redundant ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U ages in a single fossil coral fragment are possible by Multi-Collector Magnetic Sector Inductively Coupled Plasma Mass Spectrometry (MC-MS-ICPMS) and standard anion exchange column chemistry, modified to permit the separation of uranium, thorium, and protactinium isotopes from a single solution. A high-efficiency nebulizer employed for sample introduction permits the determination of both ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U ages in fragments as small as 500 mg. We have obtained excellent agreement between ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U ages in Barbados corals (30 ka) and suggest that the methods described in this paper can be used to test the ²³⁰Th/²³⁴U/²³⁸U age accuracy.Separate fractions of U, Th, and Pa are measured by employing a multi-dynamic procedure, whereby ²³⁸U is measured on a Faraday cup simultaneously with all minor isotopes measured with a Daly ion counting detector. The multi-dynamic procedure also permits correcting for both the Daly to Faraday gain and for mass discrimination during sample analyses. The analytical precision of ²³⁰Th/²³⁴U/²³⁸U and ²³¹Pa/²³⁵U dates is generally better than ±0.3% and ±1.5%, respectively (2 Relative Standard deviation [RSD]). Additional errors resulting from uncertainties in the decay constant for ²³¹Pa and from undetermined sources currently limit the ²³¹Pa/²³⁵U age uncertainty to about ±2.5%. U isotope data and ²³⁰Th/²³⁴U/²³⁸U ages agree with National Institute of Standards and Technology (NIST) reference materials and with measurements made by Thermal Ionization Mass Spectrometry (TIMS) in our laboratory.     

Ba, Ra, Th, and U in marine mollusc shells and the potential of Ra/Ba dating of Holocene marine carbonate shells

The geochemistry of Ba, Ra, Th, and U and the potential of using ²²⁶Ra/Ba ratios as an alternative dating method are explored in modern and Holocene marine mollusc shells. Five modern shells of the Antarctic scallop Adamussium colbecki collected from the present day beach and six radiocarbon dated specimens from Holocene beach terraces of the Ross Sea region (Antarctic) between 700 and 6100 calibrated yr BP old have been analysed by mass spectrometry. In clean shells ²²⁶Ra concentrations and ²²⁶Ra/Ba ratios show a clear decrease with increasing age, suggesting the possibility of ²²⁶Ra dating. Limiting factors for such dating are Ba and ²²⁶Ra present in surface contaminants, and ingrowth of ²²⁶Ra from U present within the shell. Surface contamination is difficult to clean off entirely, but moderate levels of residual contamination can be corrected using ²³²Th. Sub-samples from the same shell with different proportions of contamination form a mixing line in a ²²⁶Ra/Ba-²³²Th/Ba graph, and the ²²⁶Ra/Ba of the pure shell can be derived from the intercept on the ²²⁶Ra/Ba axis. Contaminant corrected ²²⁶Ra/Ba ratios of late-Holocene ¹⁴C-dated samples fall close to that expected from simple ²²⁶Ra excess decay from seawater ²²⁶Ra/Ba values. ²²⁶Ra ingrowth from U incorporated into the shell during the lifetime of the mollusc can be corrected for. However, the unknown timing of post mortem U uptake into the shell makes a correction for ²²⁶Ra ingrowth from secondary U difficult to achieve. In the A. colbecki shells, ²²⁶Ra ingrowth from such secondary U becomes significant only when ages exceed ∼2500 yr. In younger shells, ²²⁶Ra/Ba ratios corrected for surface contamination provide chronological information. If evidence for a constant oceanic relationship between ²²⁶Ra and Ba in the ocean can be confirmed for that time scale, the ²²⁶Ra/Ba chronometer may enable the reconstruction of variability in sea surface ¹⁴C reservoir ages from mollusc shells and allow its use as a paleoceanographic tracer.     

中国东部全新世火山的镭-钍同位素年代学

活火山是指1万年来有过喷发历史的全新世火山。火山的高分辨年代学对火山灾害评估和火山分类具有重要意义。对于缺乏历史记载的全新世火山,直接对火山岩进行同位素定年很困难。本文利用具有高时间分辨率的镭-钍-铀非平衡确定中国东部年轻火山的年龄。根据镭-钍-铀同位素,海南岛的马鞍岭和雷虎岭是全新世火山(马鞍岭:4.3ka;雷虎岭:4.7ka);镜泊湖火山(4.9ka)也是全新世火山;龙岗火山存在晚更新世和全新世活动(7.0ka,15.0ka);大兴安岭阿尔山和诺敏河Ra/Th非平衡消失但~(230)Th/~(238)U非平衡显著,属于晚更新世喷发(阿尔山:63ka;诺敏河:71ka)。海南岛的马鞍岭火山、雷虎岭火山和东北地区的龙岗火山、镜泊湖火山,是4座活火山。至于东北地区的阿尔山和诺敏河火山是否是活火山,有待测试更多样品的Ra/Th同位素。五大连池老黑山和火烧山有历史喷发记录,这与它们都存在显著Ra/Th非平衡一致。五大连池老黑山和火烧山的岩浆滞留年龄分别小于4.2ka和3.2ka,岩浆上升速率 18～23m/y。     

A new procedure for separating and measuring radiogenic isotopes (U, Th, Pa, Ra, Sr, Nd, Hf) in ice cores

A new method for the radiogenic isotope (U–Th–Pa–Ra, Sr, Nd, Hf) analysis of the soluble and insoluble components found within ice cores is presented. Melting experiments with rock standards in the presence of EDTA indicate that carbonates, as well as silicates, can be buffered sufficiently to preclude dissolution. The use of EDTA allows adsorbing species, such as Th and Hf, to remain in solution during melting thus fully separating the dust (insoluble) and sea salt (soluble) components of the ice after filtration. A new elemental separation scheme for low sample masses, less than 5 mg solid material, utilizes 4 primary ion exchange columns and two “clean-up” columns to fully isolate U, Th, Pa, Ra, Sr, Nd, and Hf while maintaining high yields. Elution schemes measured for USGS rock standards and a Chinese loess are presented to provide a comparison for variable matrix compositions. Mass spectrometer techniques were modified to measure small aliquots of the standards, equivalent to the amounts found in ice core samples, 10 ng and less. A MC-ICPMS was employed for the measurement of U, Th, Pa, Ra, and Hf; results of the experiments show that with ion yields up to 1%, rock standards have errors for ²³⁴U/²³⁸U of 1%, ²³⁰Th/²³²Th of 1.5%, [²²⁸Ra] of 9%, and ¹⁷⁶Hf/¹⁷⁷Hf of 100 ppm. MC-TIMS measurements of Sr and Nd show similar errors for small sample sizes: ⁸⁷Sr/⁸⁶Sr of 50 ppm and ¹⁴³Nd/¹⁴⁴Nd of 80 ppm. This new analytical method increases the number of possible tracers measured from a single sample, reducing separation times and sample consumption, as well as providing the addition of a radiometric clock, U-series, to the traditional suite of isotopic tracers, Sr, Nd, and Hf.     

Using short-lived nuclides of the U- and Th-series to probe the kinetics of colloid migration in forested soils

The recent chemical dynamics of a podzolic forest soil section (from the Strengbach watershed, France) was investigated using U- and Th-series nuclides. Analyses of (²³⁸U), (²³⁰Th), (²²⁶Ra), (²³²Th), (²²⁸Ra) and (²²⁸Th) activities in the soil particles, the seepage waters, and the mature leaves of the beech trees growing on this soil were performed by TIMS or gamma spectrometry. The simultaneous analysis of the different soil (sl) compartments allows to demonstrate that a preferential Th leaching over Ra must be assumed to explain the (²²⁶Ra/²³⁰Th), (²²⁸Ra/²³²Th) and (²²⁸Th/²²⁸Ra) disequilibria recorded in the soil particles. The overall Ra- and Th- transfer schemes are entirely consistent with the prevailing acido-complexolysis weathering mechanism in podzols. Using a continuous open-system leaching model, the (²²⁶Ra/²³⁰Th) and (²²⁸Ra/²³²Th) disequilibria measured in the different soil layers enable dating of the contemporary processes occurring in this soil. In this way, we have determined that a preferential Th-leaching from the shallow Ah horizon, due to a strong complexation with organic colloids, began fairly recently (18 years ago at most). The continual increase in pH recorded in precipitations over the last 20 years is assumed to be the cause of this enhanced organic complexation. A lower soil horizon (50-60 cm) is also affected by preferential Th leaching, though lasting over several centuries at least, with a much smaller leaching rate. The migration of Th isotopes through this soil section might hence be used as a tracer for the organic colloids migration and the induced radioactive disequilibria demonstrate to be useful for assessing the colloidal migration kinetics in a forested soil.Ra and Th isotopic ratios also appear to be valuable tracers of some mineral-water-plant interactions occurring in soil. The (²²⁸Ra/²²⁶Ra) ratio enables discrimination of the Ra flux originating from leaf degradation from that originating from mineral weathering in shallow −10 cm seepage soil waters. It appears that, at least in some cases, the Ra-isotopic ratio measured in forest-soil seepage waters may not be representative of the Ra-isotopic ratio released from mineral weathering, indicating that the different origins of the dissolved ²²⁶Ra and ²²⁸Ra must be taken into account.     

An improved method for Ra isotope (226Ra, 228Ra, 224Ra) measurements by gamma spectrometry in natural waters: application to CO2-rich thermal waters from the French Massif Central

An improved method was developed to measure ²²⁶Ra, ²²⁸Ra and ²²⁴Ra in freshwaters by gamma spectrometry. Radium was selectively extracted from acidified samples using specific filters (3M EMPORE™ Radium Rad disks). The latter was subsequently analysed by gamma spectrometry. Simultaneous and direct determination of the activities of the three isotopes was performed by comparison of gamma rays of the Radium Rad disks with those of a calibrated standard disk. This efficient and reliable method allowed a reduction of sample processing to a few hours.This technique was applied to analyse the Ra isotope compositions of several CO₂-rich hydrothermal springs of the western border of the Limagne graben (French Massif Central). The studied springs emerge from a succession of granitic outcrops lined up along a major fault. Their chemical compositions evolve from calcic and magnesian chloro-bicarbonated to sodic bicarbonated. All the springs display high Ra activities, probably linked to high CO₂ content and/or high cation content of these waters, with various Ra isotope ratios. ²²⁶Ra activity ranges from 588 to 2287 mBq/l and ²²⁸Ra activity from 260 to 1590 mBq/l, whereas ²²⁴Ra displays an activity between 245 and 1808 mBq/l. Four of the six analysed springs have (²²⁸Ra/²²⁶Ra) activity ratios lower than 0.7, thus, significantly lower than the ratio expected from an interaction with a calc-alkaline granitoid (typically having (²³²Th/²³⁸U) activity ratio between 1 and 2). Low (²²⁸Ra/²²⁶Ra) ratio (0.27) of the northern water (Montpensier) suggests the existence in this area of a zone of U concentration, possibly resulting from U mobilization and accumulation induced by previous hydrothermal events. The (²²⁴Ra/²²⁸Ra) ratios display smaller variations. They suggest short transit times from the zone of Ra leaching to the surface (a few days) or a very shallow addition of ²²⁴Ra (e.g., from a localised zone where ²²⁸Th could be preferentially adsorbed on the mineral surfaces). In some cases, these ratios might be used to infer differences in transit times of waters between neighboring springs.