Ion Yields in the Coupled Chemical and Physical Dynamics Model of Matrix-Assisted Laser Desorption/Ionization

Knochenmuss, Richard

doi:10.1007/s13361-015-1225-8

Cited by 17 publications

(14 citation statements)

References 33 publications

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“…This could reveal that stronger analyte/matrix interactions are promoted upon grinding the solid mixture, compared to the solvent-based sample preparation, hence accounting for incomplete evaporation of matrix molecules from MALDI clusters. Exclusive detection of covalent adducts from the "high" pressure MALDI source is however more in line with the coupled chemical and physical dynamics model proposed by Knochenmuss [30,31], with the higher MALDI plume density (compared to low pressure source) favoring interactions, and hence reactions, between matrix ions and analytes.…”

Section: Resultssupporting

confidence: 64%

Mass spectrometry of nitroxide-terminated poly(4-vinylpyridine): A case of unwanted reactive MALDI

Chendo

Phan

Marque

et al. 2016

International Journal of Mass Spectrometry

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Section: Resultssupporting

confidence: 64%

Mass spectrometry of nitroxide-terminated poly(4-vinylpyridine): A case of unwanted reactive MALDI

Chendo

Phan

Marque

et al. 2016

International Journal of Mass Spectrometry

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“…The online version of this article (https://doi.org/10.1007/s00216-020-02818-y) contains supplementary material, which is available to authorized users. fraction of desorbed molecules is ionized [6][7][8][9][10][11][12][13]. Ion yields strongly depend on the chemical properties of the matrix and the analyte itself but also on the overall composition of the sample [12,14,15].…”

Section: Electronic Supplementary Materialsmentioning

confidence: 99%

Validation of MALDI-MS imaging data of selected membrane lipids in murine brain with and without laser postionization by quantitative nano-HPLC-MS using laser microdissection

2020

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MALDI mass spectrometry imaging (MALDI-MSI) is a widely used technique to map the spatial distribution of molecules in sectioned tissue. The technique is based on the systematic generation and analysis of ions from small sample volumes, each representing a single pixel of the investigated sample surface. Subsequently, mass spectrometric images for any recorded ion species can be generated by displaying the signal intensity at the coordinate of origin for each of these pixels. Although easily equalized, these recorded signal intensities, however, are not necessarily a good measure for the underlying amount of analyte and care has to be taken in the interpretation of MALDI-MSI data. Physical and chemical properties that define the analyte molecules’ adjacencies in the tissue largely influence the local extraction and ionization efficiencies, possibly leading to strong variations in signal intensity response. Here, we inspect the validity of signal intensity distributions recorded from murine cerebellum as a measure for the underlying molar distributions. Based on segmentation derived from MALDI-MSI measurements, laser microdissection (LMD) was used to cut out regions of interest with a homogenous signal intensity. The molar concentration of six exemplary selected membrane lipids from different lipid classes in these tissue regions was determined using quantitative nano-HPLC-ESI-MS. Comparison of molar concentrations and signal intensity revealed strong deviations between underlying concentration and the distribution suggested by MSI data. Determined signal intensity response factors strongly depend on tissue type and lipid species.

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“…A two-step framework for the mechanism of MALDI has been proposed: the primary ionization step where ions are first formed during the laser pulse and the secondary reactions that follow in the desorption/ablation plume, with the first step occurring in the nanosecond timescale and the secondary reaction in the microsecond timescale [ 64 ]. While multiple models have been proposed for the ion formation in MALDI in recent years, the mechanism itself remains controversial [ [65] , [66] , [67] , [68] ].…”

Section: Basics Of Mass Spectrometrymentioning

confidence: 99%

Clinical Mass Spectrometry in the Bioinformatics Era: A Hitchhiker’s Guide

Chong

Leung

et al. 2018

Computational and Structural Biotechnology Journal

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Mass spectrometry (MS) is a sensitive, specific and versatile analytical technique in the clinical laboratory that has recently undergone rapid development. From initial use in metabolic profiling, it has matured into applications including clinical toxicology assays, target hormone and metabolite quantitation, and more recently, rapid microbial identification and antimicrobial resistance detection by matrix assisted laser desorption ionization-time of flight mass spectrometry (MALDI-TOF MS). In this mini-review, we first succinctly outline the basics of clinical mass spectrometry. Examples of hard ionization (electron ionization) and soft ionization (electrospray ionization, MALDI) are presented to demonstrate their clinical applications. Next, a conceptual discourse on mass selection and determination is presented: quadrupole mass filter, time-of-flight mass spectrometer and the Orbitrap; and MS/MS (tandem-in-space, tandem-in-time and data acquisition), illustrated with clinical examples. Current applications in (1) bacterial and fungal identification, antimicrobial susceptibility testing and phylogenetic classification, (2) general unknown urine toxicology screening and expanded new-born metabolic screening and (3) clinical metabolic profiling by gas chromatography are outlined. Finally, major limitations of MS-based techniques, including the technical challenges of matrix effect and isobaric interference; and novel challenges in the post-genomic era, such as protein molecular variants, are critically discussed from the perspective of service laboratories. Computer technology and structural biology have played important roles in the maturation of this field. MS-based techniques have the potential to replace current analytical techniques, and existing expertise and instrument will undergo rapid evolution. Significant automation and adaptation to regulatory requirements are underway. Mass spectrometry is unleashing its potentials in clinical laboratories.

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Ion Yields in the Coupled Chemical and Physical Dynamics Model of Matrix-Assisted Laser Desorption/Ionization

Cited by 17 publications

References 33 publications

Mass spectrometry of nitroxide-terminated poly(4-vinylpyridine): A case of unwanted reactive MALDI

Mass spectrometry of nitroxide-terminated poly(4-vinylpyridine): A case of unwanted reactive MALDI

Validation of MALDI-MS imaging data of selected membrane lipids in murine brain with and without laser postionization by quantitative nano-HPLC-MS using laser microdissection

Clinical Mass Spectrometry in the Bioinformatics Era: A Hitchhiker’s Guide

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