Evaluation of Matrix Effects in SIMS Using Gaussian Process Regression: The Case of Olivine Mg Isotope Microanalysis

IF 1.8 3区 化学 Q4 BIOCHEMICAL RESEARCH METHODS
Keita Itano, Kohei Fukuda, Noriko T. Kita, Kenta Ueki, Tatsu Kuwatani, Shotaro Akaho
{"title":"Evaluation of Matrix Effects in SIMS Using Gaussian Process Regression: The Case of Olivine Mg Isotope Microanalysis","authors":"Keita Itano,&nbsp;Kohei Fukuda,&nbsp;Noriko T. Kita,&nbsp;Kenta Ueki,&nbsp;Tatsu Kuwatani,&nbsp;Shotaro Akaho","doi":"10.1002/rcm.10038","DOIUrl":null,"url":null,"abstract":"<div>\n \n \n <section>\n \n <h3> Rationale</h3>\n \n <p>Matrix effects by secondary ion mass spectrometry (SIMS) are empirically corrected by calibration using matrix-matched reference materials. However, conventional parametric regression cannot estimate the prediction uncertainty to account for the difference in compositions of new data and reference materials. Applying Gaussian process regression (GPR), a nonparametric probabilistic method, enables the correction for matrix effect while providing quantitative prediction uncertainty.</p>\n </section>\n \n <section>\n \n <h3> Methods</h3>\n \n <p>We developed GPR models for estimating instrumental mass fractionation (IMF). Magnesium isotope dataset of 17 olivine reference materials was used as training data, and the developed model was applied to another data set of extraterrestrial olivines.</p>\n </section>\n \n <section>\n \n <h3> Results</h3>\n \n <p>The GPR model using FeO/MgO, CaO/MgO, Cr<sub>2</sub>O<sub>3</sub>/MgO, and MnO/MgO achieved the higher prediction accuracy of IMF (<i>R</i><sup>2</sup> = 0.98) than a previous study. We found that minor elements in olivine, such as Ca, Cr, and Mn, independently affected the matrix effect. We also demonstrated the effectiveness of this method for extraterrestrial materials.</p>\n </section>\n \n <section>\n \n <h3> Conclusions</h3>\n \n <p>We concluded that GPR is a powerful approach for correcting the SIMS matrix effect, especially when minor elements impact the matrix effect. This approach can be applied to other trace element and isotope analyses of solid-solution minerals.</p>\n </section>\n </div>","PeriodicalId":225,"journal":{"name":"Rapid Communications in Mass Spectrometry","volume":"39 13","pages":""},"PeriodicalIF":1.8000,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/rcm.10038","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Rapid Communications in Mass Spectrometry","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/rcm.10038","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"BIOCHEMICAL RESEARCH METHODS","Score":null,"Total":0}
引用次数: 0

Abstract

Rationale

Matrix effects by secondary ion mass spectrometry (SIMS) are empirically corrected by calibration using matrix-matched reference materials. However, conventional parametric regression cannot estimate the prediction uncertainty to account for the difference in compositions of new data and reference materials. Applying Gaussian process regression (GPR), a nonparametric probabilistic method, enables the correction for matrix effect while providing quantitative prediction uncertainty.

Methods

We developed GPR models for estimating instrumental mass fractionation (IMF). Magnesium isotope dataset of 17 olivine reference materials was used as training data, and the developed model was applied to another data set of extraterrestrial olivines.

Results

The GPR model using FeO/MgO, CaO/MgO, Cr2O3/MgO, and MnO/MgO achieved the higher prediction accuracy of IMF (R2 = 0.98) than a previous study. We found that minor elements in olivine, such as Ca, Cr, and Mn, independently affected the matrix effect. We also demonstrated the effectiveness of this method for extraterrestrial materials.

Conclusions

We concluded that GPR is a powerful approach for correcting the SIMS matrix effect, especially when minor elements impact the matrix effect. This approach can be applied to other trace element and isotope analyses of solid-solution minerals.

Abstract Image

理论依据 二次离子质谱法(SIMS)的基质效应是通过使用基质匹配的参照材料进行校准来进行经验校正的。然而,传统的参数回归无法估计预测的不确定性,无法考虑新数据和参考材料成分的差异。应用高斯过程回归(GPR)这种非参数概率方法,可以在提供定量预测不确定性的同时修正矩阵效应。 方法 我们开发了用于估算仪器质量分馏(IMF)的高斯过程回归模型。将 17 种橄榄石参考材料的镁同位素数据集作为训练数据,并将所开发的模型应用于另一个地外橄榄石数据集。 结果 与之前的研究相比,使用 FeO/MgO、CaO/MgO、Cr2O3/MgO 和 MnO/MgO 的 GPR 模型实现了更高的 IMF 预测精度(R2 = 0.98)。我们发现橄榄石中的次要元素(如钙、铬和锰)对基质效应有独立影响。我们还证明了这种方法对地外材料的有效性。 结论 我们得出结论,GPR 是校正 SIMS 基体效应的有力方法,尤其是当次要元素影响基体效应时。这种方法可用于固溶矿物的其他微量元素和同位素分析。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
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.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信