{"title":"Evaluation of Matrix Effects in SIMS Using Gaussian Process Regression: The Case of Olivine Mg Isotope Microanalysis","authors":"Keita Itano, Kohei Fukuda, Noriko T. Kita, Kenta Ueki, Tatsu Kuwatani, 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.
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.