Using stable oxygen isotope dual-inlet isotope-ratio mass spectrometry to elucidate uranium transport and mixed 230Th/U calcite formation ages at the seminal Devils Hole, Nevada, natural laboratory

IF 1.8 3区 化学 Q4 BIOCHEMICAL RESEARCH METHODS Rapid Communications in Mass Spectrometry Pub Date : 2024-11-23 DOI:10.1002/rcm.9926
Tyler B. Coplen, Robert R. Seal II, Lauren T. Reid, James A. Jordan, Adam C. Mumford
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Abstract

Rationale

Vein calcite in Devils Hole has been precipitating continuously in oxygen-isotope equilibrium at a constant temperature for over 500 000 years, providing an unmatched δ18O paleoclimate time series. A substantial issue is that coeval calcite (based on matching δ18O values) has uranium-series ages differing by 12 000 years.

Methods

An unparalleled high-accuracy δ18O chronology series from continuously submerged calcite was used to correct the published uranium-series ages of non-continuously formed calcite in two cores, cyclically exposed by water-table decline during glacial–interglacial transitions. This method relies on the premise that the δ18O values of coevally precipitated calcite are identical, allowing matching calcite δ18O values to establish formation ages.

Results

Exposed calcite can have apparent ages that are 12 000 years too young due to unrecognized uranium mobility and resulting mixed ages identified in over 50 mixed uranium-series ages from previous studies. Secondary uranium in fluids, sourced from the formation or dissolution of porous carbonate deposits (folia) with high uranium-238 (238U) concentrations, has migrated up to 10 mm into vein calcite.

Conclusions

The continuously submerged Devils Hole δ18O chronology is not explained by orbital forcing. Rather, this chronology represents a regional climate record in the southern Great Basin of sea-surface-temperature (SST) variations off California, variations that preceded the last and penultimate deglaciations by 5000 to approximately 10 000 years. Temporal discrepancies between the continuously submerged Devils Hole chronology and other regional δ18O records (e.g., the Leviathan chronology) can be explained by unrecognized cryptic, pernicious uranium mobility, leading to model estimations that may be thousands of years younger than actual ages. Consequently, paleo-moisture availability, water-table, and groundwater recharge models based on these mixed uranium-series ages are too young by as much as 12 000 years. The potential for post-formation uranium addition in subaerial cores and speleothems underscores the need for caution in uranium-series dating, highlighting δ18O time-series comparisons as a method for identifying mixed ages.

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利用稳定氧同位素双入口同位素比质谱法阐明内华达州魔鬼洞开创性天然实验室的铀迁移和 230Th/U 方解石混合形成年龄。
理由魔鬼洞(Devils Hole)的矿脉方解石在恒温条件下以氧同位素平衡的方式持续沉淀了 50 多万年,提供了无与伦比的 δ18O 古气候时间序列。一个重要问题是,共生方解石(基于匹配的δ18O 值)的铀系列年龄相差 12 000 年:方法:在冰川-间冰期转换过程中,水位下降周期性地暴露了两个岩心中的非连续形成的方解石,我们利用连续浸没方解石中无与伦比的高精度δ18O年代序列来校正已公布的非连续形成方解石的铀序列年龄。这种方法的前提是共同析出的方解石的 δ18O 值是相同的,这样就可以通过匹配方解石的 δ18O 值来确定形成年龄:结果:暴露的方解石的表观年龄可能比 12 000 年前太年轻,这是由于铀的流动性未得到确认,以及在以前的研究中发现的 50 多种铀系列混合年龄所导致的混合年龄。流体中的二次铀来自铀-238(238U)浓度较高的多孔碳酸盐矿床(叶片)的形成或溶解,已迁移到脉状方解石中长达 10 毫米:连续淹没的魔鬼洞δ18O年代学不能用轨道强迫来解释。相反,该年代学代表了大盆地南部的区域气候记录,即加利福尼亚附近海面温度(SST)的变化,这些变化比上一次和倒数第二次冰川期早了 5000 至约 10 000 年。连续淹没的魔鬼洞年代学与其他区域δ18O 记录(如利维坦年代学)之间的时间差异可以用未识别的隐性有害铀移动性来解释,这导致模型估计的年龄可能比实际年龄年轻数千年。因此,以这些混合铀系列年龄为基础的古湿度可用性、地下水位和地下水补给模型过于年轻,早了 12 000 年之多。在次生岩心和岩浆中可能存在形成后的铀添加,这突出表明在铀系列年代测定中需要谨慎,并强调δ18O 时间序列比较是确定混合年代的一种方法。
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来源期刊
CiteScore
4.10
自引率
5.00%
发文量
219
审稿时长
2.6 months
期刊介绍: Rapid Communications in Mass Spectrometry is a journal whose aim is the rapid publication of original research results and ideas on all aspects of the science of gas-phase ions; it covers all the associated scientific disciplines. There is no formal limit on paper length ("rapid" is not synonymous with "brief"), but papers should be of a length that is commensurate with the importance and complexity of the results being reported. Contributions may be theoretical or practical in nature; they may deal with methods, techniques and applications, or with the interpretation of results; they may cover any area in science that depends directly on measurements made upon gaseous ions or that is associated with such measurements.
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