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Application of the Sm-Nd Isotope System to the Late Quaternary Paleoceanography of the Yermak Plateau (Arctic Ocean)

机译:sm-Nd同位素体系在耶尔马克高原(北冰洋)晚第四纪古海洋学中的应用

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摘要

By storing and transporting vast amounts of energy derived from solar insolation, the oceans play an important role in shaping Earth’s climate. On the largest scale, ocean currents smooth the temperature gradients between the equator and the poles by redistributing excess energy from the tropics to higher latitudes. Much of this excess heat is transported by the so-called Ocean Conveyor Belt (Broecker, 1991), a global network of ocean currents driven by thermohaline convection. Changes in the pattern and strength of thermohaline circulation affect the redistribution of heat, and thereby significantly influence climate on local to global scales.The reconstruction of paleocurrents has long been a subject of paleoceanographic research. Among the various methods employed in tracing paleocurrents (and modern currents), the Sm-Nd isotope system is experiencing ever increasing attention. First applied in an oceanographic context by O’Nions et al. (1978), it is by now established as a standard tool, as shown by numerous recent publications (e.g. Rutberg et al., 2000; Tütken et al., 2002; Weldeab et al., 2002; Benson et al., 2003; Farmer and Barber, 2003; Piotrowski et al., 2004; Bayon et al., 2002, 2003, 2004; Lacan and Jeandel, 2001, 2004, 2005, and many more). Two lines of application of the Sm-Nd isotope system to oceanography/paleoceanography can be distinguished, both of which were followed for this thesis.The first approach uses the isotopic composition of Sm and Nd hosted in detrital minerals to infer the provenance of terrigenous sediments. This information can be used to draw conclusions about the direction and distance of sediment delivery. The second approach uses the isotopic signature of Nd as a tracer of different water masses. Due to the oceanic residence time of Nd being shorter than the global turnover rate of seawater (500-1000 years vs ~1000 years; Tachikawa et al., 2003), different bodies of water acquire distinct Nd isotopic signatures as a function of the age of adjacent continents. Apart from directly analyzing the Nd isotopic compositions of water samples to trace the modern distribution of different watermasses (e.g. Lacan and Jeandel, 2001, 2004), suitable archives of seawater-derived Nd can be employed to study paleocurrents. Possible archives are fossil remains of marine organisms (e.g. foraminifers; Burton and Vance, 2000), or, most widely used for the recent geological past, Fe-Mn nodules and crusts (e.g. Frank et al., 2002). With slow growth rates on the order of mm/Ma, however, Fe-Mn nodules do not offer the high temporal resolution necessary to study Late Quaternary climate change. Attention has therefore recently turned to authigenic Fe-Mn oxyhydroxides finely dispersed throughout the sediment column (e.g. Rutberg et al., 2000; Bayon et al., 2002, 2003, 2004; Piotrowski et al., 2004).For this thesis, both lines of application of the Sm-Nd isotope system to paleoceanography were followed. The samples were taken from a sediment core collected from the Yermak Plateau in the north-eastern Fram Strait. Situated between Greenland and the Svalbard Archipelago, the Fram Strait is the only deep connection between the Arctic Ocean and, via the Greenland-Iceland-Norwegian (Nordic) Seas, the North Atlantic. The Nordic Seas are an area of deep-water formation important for the global thermohaline circulation. There, the processes of deep-water formation are in a state of equilibrium that is most sensitive to changes in surface water salinity, which, in turn, is strongly influenced by the outflow of water of low salinity from the Arctic Ocean. This makes the history of water exchange between the Atlantic and the Arctic Ocean through the Fram Strait a subject of key interest for climate research.In particular, it was attempted to reconstruct the provenance of sediments deposited on the western Yermak Plateau over the last 129 000 years. This was done by analyzing samples from the sediment core and from potential source areas for their Sm-Nd isotopic compositions. The current understanding is that under present interglacial conditions sediment is delivered to the Yermak Plateau by ice drift from the Siberian shelf areas (Kara- and Laptev Sea) and as suspended load of Atlantic water advected from the south. To resolve these assumed differences in provenance and transport mechanism, the majority of the samples was split into the grain-size fractions clay, fine silt, coarse silt, and sand for Sm-Nd analyses. The position of the investigated core on the upper slope of the western Yermak Plateau limits delivery of sand-size (or coarser) material to ice rafting. The sand fractions of the core samples were therefore interpreted to be exclusively of ice rafted origin, and thus used as an indicator of changes in the pattern of surface currents. Clay- to silt-size material, on the other hand, yields a mixed signal of ice rafting and suspended-load delivery. Based on a comparison of the isotopic compositions of the core samples with those of the samples from potential source areas, a number of conclusions can be drawn: Most core sample show only little isotopic variation between their constituent size fractions (mostly less than analytical uncertainty). Only sand fractions show considerable differences. This can probably be explained by the sand samples’ small sample size relative to their coarse grain size; as a result, most sand fractions probably are not representative.The generally good agreement between the isotopic compositions suggests a common origin of ice rafted detritus (IRD) and suspended load. The possibility of suspended particulate matter transport from the Siberian shelf areas of the Kara- and Laptev Seas to the Yermak Plateau in significant amounts can be excluded. An origin of IRD in the Kara and Laptev Sea is therefore equally unlikely. Instead, a common provenance of IRD and suspended particulate matter from the Svalbard/Barents Sea area is a plausible scenario, supported by isotope-independent data from the literature (e.g. grain-size distribution, mineralogical composition, faunal abundance, etc.).The moderate downcore Nd isotopic variation suggests that, despite repeated large-scale glaciations in the Svalbard/Barents Sea area, the general modern-type circulation in the Fram Strait area has been active for most of the last 129 000 years. The largest deviation from modern conditions is indicated for the peak of the last glacial phase, approximately 20 000 years ago. Then, large amounts of IRD were delivered to the Yermak Plateau by icebergs calving from the Scandinavian ice sheet. Moreover, the occurrence of chalk fragments confirms iceberg drift from as far south as the North Sea. A similar finding has previously been reported for samples from the southern Fram Strait by Spielhagen (1991).Regarding the second analytical approach, i.e. the Nd isotopic analysis of finely dispersed authigenic Fe-Mn oxyhydroxides, implementation of the experimental technique was targeted first. The method of Fe-Mn oxyhydroxide extraction by means of leaching with a mixed reagent (acetic acid and hydroxylamine-hydrochloride) largely is based on the work of Chester and Hughes (1967). Modifications of their method have been reported in Tessier et al. (1979), Chao and Zhou (1983), and Hall et al. (1996), and have recently been compared by Bayon et al. (2002). Based on the experimental protocol described by Bayon et al. (2002), five core samples were processed and analyzed for their rare earth element (REE) concentrations by ICP-MS at the European Union Large Scale Geochemical Facility at the University of Bristol, England, financed by the EU. In addition, nine core samples were processed and the leachates analyzed for their Nd isotopic composition in Munich.The REE patterns of the leachates show an enrichment of the middle REE that is atypical for authigenic Fe-Mn phases. The isotopic analysis also yielded controversial results: downcore, the Nd isotope curves for the leachates and the detrital phases run approximately parallel, suggesting a systematic genetic relationship between the analyzed Nd fractions. A similar relationship appears to exist between data reported in Rutberg (2000), Rutberg et al. (2000), and Piotrowski et al. (2004) for a sediment core from the south-eastern Atlantic.To answer the questions raised by these controversial results, a sequential leaching experiment was designed. Several aliquots of one core sample were treated for different durations with different concentrations of the leaching reagents, and at intermediate steps were analyzed for their Sm-Nd isotopic composition. The results of this leaching experiment point towards a conceptual weakness of the method. In order to avoid contamination by non-authigenic sediment components, all experimental methods described in the literature focus on adjusting the concentration of the hydroxylamine-hydrochloride used to reduce Fe and Mn to their soluble states. This approach, however, does not take into account the dissolution of acid-soluble phases by acetic acid, which in all cases is used at a strength of 4.4 mol·l-1. Consequently, the leaching reagent is sufficiently corrosive to attack easily-soluble detrital minerals and release non-seawater-derived Nd (Hannigan and Sholkovitz, 2001; Dubinin and Strekopytov, 2001). Phosphatic phases are therefore a likely source of nonseawater-derived Nd. Apatite, for instance, is a common component of clastic sedimentary rocks, is easily dissolved by weak acids, and can account for the middle REE enrichment in the leachates. Its high Nd concentrations would mask any seawater signal. To conclude, it appears as though the available extraction techniques are not yet sufficiently refined to reliably determine the Nd isotopic composition of finely dispersed Fe-Mn oxyhydroxides as a proxy for paleoseawater composition.
机译:通过储存和运输来自日照的大量能量,海洋在塑造地球气候方面发挥着重要作用。在最大的范围内,洋流通过将多余的能量从热带重新分配到较高的纬度来平滑赤道和两极之间的温度梯度。多余的热量大部分由所谓的海洋输送带(Broecker,1991)输送,这是由热盐对流驱动的全球洋流网络。热盐循环模式和强度的变化会影响热量的重新分布,从而在局部到全球范围内显着影响气候。古电流的重建长期以来一直是古海洋学研究的主题。在追踪古电流(和现代电流)的各种方法中,Sm-Nd同位素系统受到越来越多的关注。 O’Nions等人首次将其应用于海洋环境。 (1978年),它已被确立为一种标准工​​具,如最近的许多出版物所示(例如Rutberg等,2000;Tütken等,2002; Weldeab等,2002; Benson等,2003; Waldeab等,2002)。 Farmer和Barber,2003; Piotrowski等,2004; Bayon等,2002,2003,2004; Lacan和Jeandel,2001,2004,2005等。可以区分Sm-Nd同位素系统在海洋学/古海洋学中的两种应用,这两种方法均适用于本论文。第一种方法是利用碎屑矿物中Sm和Nd的同位素组成推断陆源沉积物的来源。该信息可用于得出有关沉积物输送方向和距离的结论。第二种方法使用Nd的同位素特征作为不同水团的示踪剂。由于Nd在海洋中的停留时间短于全球海水的周转率(500-1000年对〜1000年; Tachikawa等人,2003年),不同的水体随着年龄的增长而获得独特的Nd同位素特征。相邻大陆。除了直接分析水样品的Nd同位素组成以追踪不同水质的现代分布外(例如Lacan和Jeandel,2001,2004),还可以采用海水衍生Nd的合适档案来研究古流。可能的档案是海洋生物的化石遗骸(例如有孔虫; Burton和Vance,2000年),或者在最近的地质历史中使用最广泛的Fe-Mn结节和地壳(例如Frank等人,2002年)。然而,由于缓慢的生长速度在毫米/马的数量级,铁锰结核没有提供研究晚第四纪气候变化所必需的高时间分辨率。因此,近来关注的是细微分散在整个沉积物中的自生Fe-Mn羟基氧化物(例如Rutberg等,2000; Bayon等,2002,2003,2004; Piotrowski等,2004)。遵循Sm-Nd同位素系统在古海洋学中的应用路线。样品取自弗拉姆海峡东北部的叶尔马克高原的沉积物岩心。弗兰姆海峡位于格陵兰岛和斯瓦尔巴群岛之间,是北冰洋与格陵兰岛,冰岛,挪威(北欧)海以及北大西洋之间的唯一深层连接。北欧海域是深水形成区域,对全球热盐环流至关重要。那里,深水形成过程处于平衡状态,该状态对地表水盐度的变化最敏感,反过来,低盐度水从北冰洋流出的影响很大。这使得通过弗拉姆海峡在大西洋和北冰洋之间进行水交换的历史成为气候研究的重要课题,尤其是试图重建过去129 000年沉积在西尔马克高原西部的沉积物来源年份。这是通过分析沉积物核心和潜在源区的Sm-Nd同位素组成的样品来完成的。目前的理解是,在目前的冰间条件下,沉积物通过从西伯利亚陆架地区(卡拉和拉普捷夫海)的冰漂流以及从南方平流的大西洋水的悬浮物而被输送到亚尔马克高原。为了解决这些原产地和运输机制的假设差异,将大多数样品分为粒度级分的粘土,细粉砂,粗粉砂和沙子,以进行Sm-Nd分析。被调查的岩心在叶尔马克高原西部较高坡度上的位置限制了将沙粒(或更粗)材料运送到冰上漂流。因此,岩心样品的砂级分被解释为仅是漂流冰的来源,因此可以用作表面流模式变化的指标。另一方面,粘土到淤泥大小的材料,会产生冰上漂流和悬浮负载传递的混合信号。根据核心样品的同位素组成与潜在来源地区的同位素组成的比较,可以得出以下结论:大多数核心样品在其组成尺寸分数之间仅表现出很小的同位素变化(大多数小于分析不确定度) 。只有沙子部分显示出相当大的差异。这可能是由于沙粒样本相对于粗粒样本的样本量较小而造成的。结果,大多数沙子组分可能没有代表性。同位素组成之间的总体良好一致性表明,浮冰碎屑(IRD)和悬浮负荷是常见的。可以排除悬浮颗粒物从卡拉海和拉普捷夫海的西伯利亚陆架区域大量运输到叶尔马克高原的可能性。因此,IRD起源于卡拉和拉普捷夫海的可能性也不大。取而代之的是,IRD和来自斯瓦尔巴特/巴伦支海地区的悬浮颗粒物的共同来源是一个合理的情况,并得到了文献中与同位素无关的数据(例如晶粒大小分布,矿物组成,动物群落丰度等)的支持。温和的下层Nd同位素变化表明,尽管斯瓦尔巴特/巴伦支海地区反复出现大型冰川,但在过去129 000年的大部分时间里,弗拉姆海峡地区的现代现代环流一直活跃。与现代条件的最大偏差显示在大约2万年前的最后一个冰川期的高峰期。然后,大量的IRD通过从斯堪的纳维亚冰盖上裂下的冰山传递到了Yermak高原。此外,白垩碎片的出现证实了冰山从最南端到北海的漂流。 Spielhagen(1991)以前从南弗拉姆海峡的样品中也报道了类似的发现,关于第二种分析方法,即对细分散的自生Fe-Mn羟基氧化物进行Nd同位素分析,首先针对的是实验技术的实现。通过用混合试剂(乙酸和盐酸羟胺)浸出的方法提取Fe-Mn羟基氧化物的方法主要是基于Chester和Hughes(1967)的工作。 Tessier等人已经报道了他们方法的改进。 (1979),Chao and Zhou(1983)和Hall等。 (1996年),最近被Bayon等人进行了比较。 (2002)。根据Bayon等人描述的实验方案。 (2002年),由英国资助,由英国布里斯托大学的欧盟大型地球化学工厂的ICP-MS对五个核心样品进行了处理,并分析了它们的稀土元素(REE)浓度。此外,在慕尼黑对9个岩心样品进行了处理,并对渗滤液的Nd同位素组成进行了分析。渗滤液的REE模式显示出中生REE的富集,这是非自生的Fe-Mn相的典型特征。同位素分析也产生了有争议的结果:下限,浸出液的Nd同位素曲线和碎屑相大致平行,这表明分析的Nd组分之间存在系统的遗传关系。在Rutberg(2000),Rutberg等人(2000)报道的数据之间似乎存在相似的关系。 (2000)和Piotrowski等。为了解决这些有争议的结果提出的问题,我们设计了一个连续浸出实验(2004年),该实验来自大西洋东南部。一个核心样品的几个等分试样用不同浓度的浸出试剂处理不同的持续时间,并在中间步骤分析其Sm-Nd同位素组成。该浸出实验的结果表明该方法在概念上存在缺陷。为了避免被非自生的沉积物成分污染,文献中描述的所有实验方法都集中在调节用于将Fe和Mn还原为其可溶态的羟胺盐酸盐的浓度。但是,该方法未考虑乙酸对酸溶相的溶解,在所有情况下,乙酸的溶解强度为4.4mol·l-1。因此,该浸出剂具有足够的腐蚀性,可侵蚀易溶的碎屑矿物并释放非海水衍生的Nd(Hannigan和Sholkovitz,2001; Dubinin和Strekopytov,2001)。因此,磷相可能是非海水来源的钕的来源。例如,磷灰石是碎屑沉积岩的常见成分,很容易被弱酸溶解,并且可以解释渗滤液中稀土元素的富集。它的高Nd浓度会掩盖任何海水信号。总结一下,似乎可用的提取技术尚未充分完善,无法可靠地确定精细分散的Fe-Mn羟基氧化物的Nd同位素组成,以代替古水成分。

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    Schmitt Wolfgang;

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