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同位素双稀释剂技术的数值模拟与应用 被引量:5

The numerical optimization of isotope double spike and its applications
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摘要 近年来,非传统稳定同位素地球化学已成为新兴发展的研究领域,同位素双稀释剂技术是该领域的主流分析方法之一,但始终存在的困扰问题是如何进行同位素双稀释剂间以及稀释剂与样品间的最优混合。这两种混合比严重制约着同位素比值测试的准确度、精度和重现性。本文从同位素双稀释剂技术的数学原理出发,以Cr、Mo同位素为例,结合MonteCarlo误差模型,深入讨论和分析了两单稀释剂间比值(λ)及双稀释剂与自然样品间比值(p)的最优化数值模拟,得到了以双稀释剂~50(Cr)-~54(Cr)、~97(Mo)-^(100)Mo为例的λ、p值的最优取值范围。该数值模拟可适用于所有能够利用同位素双稀释剂技术的元素。在此基础上,就数值模拟结果如何应用于同位素双稀释剂的选择和组成标定也给予了详细说明,这为我国开展和使用同位素双稀释剂技术提供了基本思路和需要注意的关键问题,有助于推动同位素双稀释剂技术在我国地学界的广泛应用和发展。 In recent years, the geochemistry of non-traditional stable isotopes is developing to be a novel studying field. The isotope double spike technique has been becoming one of the main analytical methods in determining isotopic composition. However, the always perplexing problem for researchers is of how to get the best mixing proportion between the two single spikes (λ), and the optimal mixing ratio for the double spike and sample (p). These two parameters severely restrict the accuracy, precision and the long reproducibility of the isotopes measurement. In this paper, we systematically elaborated on the mathematical principle of double spike technique as an example of chromium (Cr) and molybdenum (Mo) isotopes, and further discussed the numerical simulation optimization for getting above two parameters combined with the Monte-Carlo error model. The optimal simulated ratios of λ and p for 50Cr-54Cr and 97Mo-100Mo double spike are presented. The case study showed that this numerical simulation method for double spike can be applied to all elements with 4 or more isotopes. On the basis of the above, we presented the detailed description of how to use the numerical optimization results of double spike to select and calibrate double spike. Meanwhile, some trouble issues and the basic routine during using double spike are also presented for researchers who will engage in double spike. This paper will be helpful to promote the development of double spike and its extensively application in Chinese geosciences community.
出处 《岩石学报》 SCIE EI CAS CSCD 北大核心 2018年第2期503-512,共10页 Acta Petrologica Sinica
基金 本文受国家重点基础研究发展规划(2014CB238903)和国家自然科学基金项目(41473028、41273029、41073017)联合资助.本文工作的完成和发表得益于美国伊利诺伊大学香槟分校地质系Johnson教授、中国科学院地质与地球物理所吴福元研究员的鼓励和讨论,也得到中国地质科学院地质研究所朱祥坤研究员、中国科学院广州地球化学研究所张兆峰研究员、德国马普研究所Galer博士、英国剑桥大学Rudge博士以及两位匿名审稿人的建议和帮助,谨此致谢.致谢本文工作的完成和发表得益于美国伊利诺伊大学香槟分
关键词 同位素双稀释剂法 数值模拟优化 Monte-Carlo误差模型 CR MO同位素 Double spike technique Numerical optimization Monte Carlo error model Cr and Mo isotopes
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