{"title":"提高LA-ICP-MS元素成像空间精度的数值反演新方法","authors":"Yuan Hu, Zhaochu Hu, Wen Zhang","doi":"10.1021/acs.analchem.4c06214","DOIUrl":null,"url":null,"abstract":"The elemental imaging of laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) provides spatial information on elements and therefore can further investigate the growth or evolution processes of an analyte. However, the accurate determination of spatial information is limited by the decoupling between the elemental distribution and mass spectrometry signals. This phenomenon, which is more distinct when high-diffusion ablation cells are used, arises from the overlap of ablation and the transport dispersion of aerosols. Reconstruction of the elemental distribution using mathematical algorithms is an effective approach to addressing this decoupling. This study establishes a comprehensive numerical inversion method that targets the independent events of aerosol diffusion and overlapping ablation in LA-ICP-MS. A new signal fitting model and deconvolution algorithm are employed to mitigate the effects of aerosol diffusion. Moreover, boundary identification and restoration algorithms are developed to resolve the challenges posed by blurring of the phase boundary when the laser beam scans over the two-phase interface. By employing the presented numerical method, the shape of fine materials can be measured with an accuracy of 10%, which is an ∼18-fold improvement compared to the raw data. The new algorithm is expected to enhance the accuracy of the spatial distribution in LA-ICP-MS elemental imaging, particularly for traditional high-diffusion ablation cells, which are still in use in microanalytical laboratories on a global scale. Additionally, the numerical inversion method presented here can be applied across various fields of science to improve the quality of element imaging.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"37 1","pages":""},"PeriodicalIF":6.7000,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"New Numerical Inversion Method to Improve the Spatial Accuracy of Elemental Imaging for LA-ICP-MS\",\"authors\":\"Yuan Hu, Zhaochu Hu, Wen Zhang\",\"doi\":\"10.1021/acs.analchem.4c06214\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The elemental imaging of laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) provides spatial information on elements and therefore can further investigate the growth or evolution processes of an analyte. However, the accurate determination of spatial information is limited by the decoupling between the elemental distribution and mass spectrometry signals. This phenomenon, which is more distinct when high-diffusion ablation cells are used, arises from the overlap of ablation and the transport dispersion of aerosols. Reconstruction of the elemental distribution using mathematical algorithms is an effective approach to addressing this decoupling. This study establishes a comprehensive numerical inversion method that targets the independent events of aerosol diffusion and overlapping ablation in LA-ICP-MS. A new signal fitting model and deconvolution algorithm are employed to mitigate the effects of aerosol diffusion. Moreover, boundary identification and restoration algorithms are developed to resolve the challenges posed by blurring of the phase boundary when the laser beam scans over the two-phase interface. By employing the presented numerical method, the shape of fine materials can be measured with an accuracy of 10%, which is an ∼18-fold improvement compared to the raw data. The new algorithm is expected to enhance the accuracy of the spatial distribution in LA-ICP-MS elemental imaging, particularly for traditional high-diffusion ablation cells, which are still in use in microanalytical laboratories on a global scale. Additionally, the numerical inversion method presented here can be applied across various fields of science to improve the quality of element imaging.\",\"PeriodicalId\":27,\"journal\":{\"name\":\"Analytical Chemistry\",\"volume\":\"37 1\",\"pages\":\"\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2025-01-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Analytical Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.analchem.4c06214\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytical Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.analchem.4c06214","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
New Numerical Inversion Method to Improve the Spatial Accuracy of Elemental Imaging for LA-ICP-MS
The elemental imaging of laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) provides spatial information on elements and therefore can further investigate the growth or evolution processes of an analyte. However, the accurate determination of spatial information is limited by the decoupling between the elemental distribution and mass spectrometry signals. This phenomenon, which is more distinct when high-diffusion ablation cells are used, arises from the overlap of ablation and the transport dispersion of aerosols. Reconstruction of the elemental distribution using mathematical algorithms is an effective approach to addressing this decoupling. This study establishes a comprehensive numerical inversion method that targets the independent events of aerosol diffusion and overlapping ablation in LA-ICP-MS. A new signal fitting model and deconvolution algorithm are employed to mitigate the effects of aerosol diffusion. Moreover, boundary identification and restoration algorithms are developed to resolve the challenges posed by blurring of the phase boundary when the laser beam scans over the two-phase interface. By employing the presented numerical method, the shape of fine materials can be measured with an accuracy of 10%, which is an ∼18-fold improvement compared to the raw data. The new algorithm is expected to enhance the accuracy of the spatial distribution in LA-ICP-MS elemental imaging, particularly for traditional high-diffusion ablation cells, which are still in use in microanalytical laboratories on a global scale. Additionally, the numerical inversion method presented here can be applied across various fields of science to improve the quality of element imaging.
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.