Improving detection thresholds and robust event filtering in single-particle and single-cell ICP-MS analysis

Literature Information

Publication Date 2023-10-30
DOI 10.1039/D3JA00292F
Impact Factor 4.023
Authors

Matthias Elinkmann, Sarah Reuter, Michael Holtkamp, Steffen Heuckeroth, Alexander Köhrer, Katharina Kronenberg, Michael Sperling, Oliver Rubner, C. Derrick Quarles, Jr, Michael Hippler, Uwe Karst


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Abstract

In this work, a modular data processing workflow for single-particle (sp) and single-cell (sc) inductively coupled plasma-mass spectrometry (ICP-MS) is presented. To achieve more reliable detection thresholds, a special focus is placed on the parameter estimation of Gaussian and Poisson distributions that describe the background (BG) signal. For Gaussian models, the widely used iterative outlier test was improved by an algorithm that adjusts the test for different BG levels by incrementing the test factor. Through careful evaluation, the standard deviation of the experimental sc- and sp-ICP-MS data was applied as a robust measure of the convergence quality of the test. In addition, the outlier analysis was separated from the subsequent event detection more strictly than it is often reported. Importantly, a data-dependent decision criterion based on Gaussian and Poisson modeling was developed to effectively address extra-Poisson variance in experimental data. In the second part, a gate filter was developed to reduce the amount of excess false-positive events in sc-ICP-MS. To that end, a secondary filter based on the signal peak height is used to remove rare false-positive events without affecting the signal intensity of the events that are detected correctly. Two approaches, based on a numerical approximation via the detection limit, and critical values of the Gaussian and Poisson distribution are presented to calculate the gate filter level. Possible sources of false-positive events, some of which are specific to sc-ICP-MS, are discussed. The combined processing workflow was applied to analyze the distribution of six endogenous elements in Chlamydomonas reinhardtii cell populations. The gate filter corrected the cell number concentration by up to 44% (22% on average), and mass per cell by up to 30% (17% on average).

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Journal of Analytical Atomic Spectrometry

Journal of Analytical Atomic Spectrometry
CiteScore: 6.2
Self-citation Rate: 25.8%
Articles per Year: 254

The Journal of Analytical Atomic Spectrometry (JAAS) is the central journal for publishing innovative research on fundamentals, instrumentation, and methods in the determination, speciation and isotopic analysis of (trace) elements within all fields of application. This includes, but is not restricted to, the most recent progress, developments and achievements in all forms of atomic and elemental detection, isotope ratio determination, molecular analysis, plasma-based analysis and X-ray techniques. The journal welcomes full papers, communications, technical notes, critical and tutorial review articles, editorials, and comments, in addition to the Atomic Spectrometry Updates (ASU) literature reviews that are prepared by an expert panel. Submissions are welcome in the following areas, but note this list reflects the current scope and authors are strongly encouraged to contact the Editorial team if they believe that their work offers potentially new and emerging research relevant to the journal remit: Fundamental studies in the following. New and existing sources for atomic emission, absorption, fluorescence and mass spectrometry and those that provide both atomic and molecular information Sample introduction techniques for solids, liquids, gases Improvements in sensitivity, selectivity, precision, accuracy and/or robustness Isotope ratio measurements, including techniques for improving precision and mass bias correction Single channel and multichannel simultaneous detection systems Chemometrics, statistics, calibration techniques and internal standardisation Theoretical and numerical modelling of fundamental processes related to all of the above methodologies Novel or improved methodologies in areas of application including, but not limited to the following. Biosciences, including elemental, speciation and isotopic analysis in biological systems, immunoassays based on metal-labeled antibodies, bio-imaging, and nanoparticle toxicology Geochemistry Environmental science Materials science, including engineered nanoparticles and quantum dots Metrology, including reference materials Forensic analysis Food and agricultural sciences Energy Archaeometry Molecular analysis. Molecular sources for elemental and isotopic analysis Atomic sources for molecular analysis Atomic and molecular techniques simultaneously used for complementary chemical information All contributions are judged on originality and quality of scientific content, and appropriateness of length to content of new science.

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