Cryo laser-ablation system (157+193nm) with 'triple-quad' plasma mass spectrometer, Cryo-LA-ICPMS/MS

我们请求为一个双波长(157+193 nm)冷冻激光消融系统和一个三重四极等离子质谱仪提供资金，这两个系统将在德国和世界范围内形成一个分析设备，即具有独特分析能力的CRYO-LA-ICPMS/MS。该激光系统的主要创新包括最新研制的大冷冻双体积激光加速器和两个可交替使用的超短准分子激光光源组合，即157 nm和193 nm。超短的157 nm波长对冰的吸收提高了约10个数量级，这显著改善了冰的LA，特别是在低气溶胶浓度的情况下，而更大的LA池则允许对长冰芯切片的研究。结合LA池的快速清洗漏斗和高激光频率，快速2D映射将成为可能。“三重四极”等离子质谱仪是与Cryo-LA系统并驾齐驱的另一个重要部件。高灵敏度、前所未有的丰度灵敏度和质量选择性(例如，当m/z=87或32时)，以及快速扫描(&gt；100微米S)在质谱图中的组合，使非常通用的分析可能性成为可能。新的CRYO-LA-ICPMS/MS系统开辟了一系列前所未有的研究领域：显著提高的空间分辨率(相对于连续流动分析)导致了更深、更薄的冰芯更好的年度时间分辨率。我们计划系统地阐明格陵兰冰芯(Dansgaard-Oeschger-EV.)气候突变事件的动力学。通过重建冷/暖过渡期间的大气(尘埃)动力学。最终，这将使我们能够确定自然气候变化的速度。我们计划通过现场硫(同位素)分析重建火山喷发及其大气范围(例如，特罗波与平流层)。(尘埃)气溶胶在冰芯中自然重结晶颗粒中的行为，或在冷冻组织样本上的生物应用是进一步的途径。Rb/Sr原位测年将是进一步的关键发展，例如应用于基质中的变质白云母与包裹体，以确定进变质作用或变形事件的日期。同样，碎屑白云母测年将被用来重建过去类似于锆石中U/Pb的沉积源区。Sylvin是Rb/Sr原位测年的一个重要目标，因为它与核废料储存库的设计有关。通过电感耦合等离子体质谱(ICMS/MS)的高丰度灵敏度，原位U/Th不平衡测年，例如晚更新世骨骼或牙本质的铀摄取模型，是可能的。我们计划系统地评估硫酸盐、硫酸盐、石英砂或碳酸盐等难烧蚀矿物的157 nm与193 nm LA的对比。威士的工作人员在LA-ICPMS仪器的设计、安装和操作方面拥有数十年的经验，特别是在Cryo-LA和ICP-MS/MS方面，因此他们非常适合实施Cryo-157-193 nm LA-ICPMS/MS。

We request funding for a dual wavelength (157+193 nm) cryo-laser-ablation system and a triple quadrupole plasma mass spectrometer, which together will form one analytical device, a cryo-LA-ICPMS/MS, with unique analytical capabilities - in Germany and worldwide. The main innovations of this LA system include a newly-developed large cryo-two-volume LA cell and the combination of two ultrashort excimer laser sources, namely 157 nm wavelength and 193 nm, which can be used alternatively. The ultrashort 157 nm wavelength shows ~10 orders of magnitude better absorption for ice, which significantly improves LA of ice especially with low aerosol concentrations, while the larger LA cell allows investigations of long ice core sections. In combination with the fast washout funnel of the LA cell and high laser frequencies, rapid 2D mapping will be possible. The 'triple quadrupole' plasma mass spectrometer is the other essential component alongside the cryo-LA system. The combination of high sensitivity, unprecedented abundance sensitivity and mass selectivity (e.g. for m/z=87 or 32), as well as fast scanning (>100 µs) through the mass spectrum enables extremely versatile analytical possibilities. The new cryo-LA-ICPMS/MS system opens up an unprecedented array-of research areas: The significantly improved spatial resolution (relative to continuous flow analysis) results in better-than-annual time resolution in deep, thinned ice cores. We plan to systematically elucidate the dynamics of Abrupt Climate Change events in Greenland ice cores (Dansgaard-Oeschger-ev.) via reconstructions of atmospheric (dust) dynamics during cold/warm transitions. Ultimately this should allow us to determine rates of natural climate change. We plan to reconstruct volcanic eruptions and their atmospheric extent (e.g. tropo vs. stratosphere) by means of in-situ sulphur (isotopic) analysis. The behaviour of (dust) aerosols in naturally-recrystallising grains in ice cores, or biological applications on frozen tissue samples are further avenues. In-situ Rb/Sr dating will be a further key development, e.g. applied to metamorphic white mica in matrix vs. inclusions to date prograde metamorphism, or deformation events. Equally, dating of detrital white mica will be used to reconstruct past sedimentary source areas analogous to U/Pb in zircons. Sylvin is an important target for in-situ Rb/Sr dating, as it is relevant for nuclear waste repository design. In-situ U/Th disequilibrium dating, e.g. of late Pleistocene bone or dentin combined with U uptake modelling, is possible via the high abundance sensitivity of ICP-MS/MS. We plan to systematically evaluate comparative 157 nm vs. 193 nm LA for difficult-to-ablate minerals such as sulphates, sylvin, quartz or carbonates. The staff at FIERCE have decades of experience in the design, setup and operation of LA-ICPMS instruments, especially also with cryo-LA and ICP-MS/MS, and are therefore well-placed to implement cryo-157-193 nm LA-ICP-MS/MS.