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首页> 美国卫生研究院文献>Proceedings of the National Academy of Sciences of the United States of America >Ultra-high-resolution paleoenvironmental records via direct laser-based analysis of lipid biomarkers in sediment core samples
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Ultra-high-resolution paleoenvironmental records via direct laser-based analysis of lipid biomarkers in sediment core samples

机译：通过直接基于激光的沉积物岩心样品中脂质生物标志物分析获得超高分辨率的古环境记录

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Marine microorganisms adapt to their habitat by structural modification of their membrane lipids. This concept is the basis of numerous molecular proxies used for paleoenvironmental reconstruction. Archaeal tetraether lipids from ubiquitous marine planktonic archaea are particularly abundant, well preserved in the sedimentary record and used in several molecular proxies. We here introduce the direct, extraction-free analysis of these compounds in intact sediment core sections using laser desorption ionization (LDI) coupled to Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). LDI FTICR-MS can detect the target lipids in single submillimeter-sized spots on sediment sections, equivalent to a sample mass in the nanogram range, and could thus pave the way for biomarker-based reconstruction of past environments and ecosystems at subannual to decadal resolution. We demonstrate that ratios of selected archaeal tetraethers acquired by LDI FTICR-MS are highly correlated with values obtained by conventional liquid chromatography/MS protocols. The ratio of the major archaeal lipids, caldarchaeol and crenarchaeol, analyzed in a 6.2-cm intact section of Mediterranean sapropel S1 at 250-µm resolution (∼4-y temporal resolution), provides an unprecedented view of the fine-scale patchiness of sedimentary biomarker distributions and the processes involved in proxy signal formation. Temporal variations of this lipid ratio indicate a strong influence of the ∼200-y de Vries solar cycle on reconstructed sea surface temperatures with possible amplitudes of several degrees, and suggest signal amplification by a complex interplay of ecological and environmental factors. Laser-based biomarker analysis of geological samples has the potential to revolutionize molecular stratigraphic studies of paleoenvironments.
机译：海洋微生物通过膜脂的结构修饰来适应其栖息地。该概念是用于古环境重建的众多分子代理的基础。来自无处不在的海洋浮游古细菌的古生四醚脂质​​特别丰富，在沉积记录中保存得很好，并用于多种分子代理中。我们在此介绍使用激光解吸电离（LDI）与傅立叶变换离子回旋共振质谱（FTICR-MS）耦合的完整沉积物岩心部分中这些化合物的直接，无萃取分析。 LDI FTICR-MS可以检测沉积物截面上单个亚毫米大小的斑点中的目标脂质，相当于纳克范围内的样品质量，从而可以为基于生物标志物的过去一年到十年分辨率的过去环境和生态系统重建铺平道路。我们证明了通过LDI FTICR-MS获得的所选古细菌四醚的比例与通过常规液相色谱/ MS协议获得的值高度相关。在地中海腐殖质S1的6.2厘米完整部分中以250 µm分辨率（约4 y时间分辨率）分析了主要古生类脂质，去甲酚和地雷烯酚的比率，这为沉积物的细小斑块提供了前所未有的视角生物标志物分布和代理信号形成过程。脂质比率的时间变化表明200 y de Vries太阳周期对重构海面温度的强烈影响，幅度可能为几度，并暗示由于生态和环境因素之间复杂的相互作用而导致信号放大。基于激光的地质样品生物标记分析有可能彻底改变古环境的分子地层学研究。

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