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      (CO 2) n +, (H 2O) n +, and (H 2O) n + (CO 2) gas cluster ion beam secondary ion mass spectrometry: analysis of lipid extracts, cells, and Alzheimer’s model mouse brain tissue

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          Graphical abstract

          This work assesses the potential of new water cluster-based ion beams for improving the capabilities of secondary ion mass spectrometry (SIMS) for in situ lipidomics. The effect of water clusters was compared to carbon dioxide clusters, along with the effect of using pure water clusters compared to mixed water and carbon dioxide clusters. A signal increase was found when using pure water clusters. However, when analyzing cells, a more substantial signal increase was found in positive ion mode when the water clusters also contained carbon dioxide, suggesting that additional reactions are in play. The effects of using a water primary ion beam on a more complex sample were investigated by analyzing brain tissue from an Alzheimer’s disease transgenic mouse model. The results indicate that the ToF-SIMS results are approaching those from MALDI as ToF-SIMS was able to image lyso-phosphocholine (LPC) lipids, a lipid class that for a long time has eluded detection during SIMS analyses. Gangliosides, sulfatides, and cholesterol were also imaged.

          Supplementary Information

          The online version contains supplementary material available at 10.1007/s00216-021-03372-x.

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          Most cited references53

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          Mass spectrometry sampling under ambient conditions with desorption electrospray ionization.

          Zoltan Takats, Justin M Wiseman, Bogdan Gologan … (2004)
          A new method of desorption ionization is described and applied to the ionization of various compounds, including peptides and proteins present on metal, polymer, and mineral surfaces. Desorption electrospray ionization (DESI) is carried out by directing electrosprayed charged droplets and ions of solvent onto the surface to be analyzed. The impact of the charged particles on the surface produces gaseous ions of material originally present on the surface. The resulting mass spectra are similar to normal ESI mass spectra in that they show mainly singly or multiply charged molecular ions of the analytes. The DESI phenomenon was observed both in the case of conductive and insulator surfaces and for compounds ranging from nonpolar small molecules such as lycopene, the alkaloid coniceine, and small drugs, through polar compounds such as peptides and proteins. Changes in the solution that is sprayed can be used to selectively ionize particular compounds, including those in biological matrices. In vivo analysis is demonstrated.
          Article 0 comments Cited 226 times – based on 0 reviews     Review now
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            Molecular imaging of biological samples: localization of peptides and proteins using MALDI-TOF MS.

            Richard M. Caprioli, Terry B. Farmer, Jocelyn Gile (1997)
            Matrix-assisted laser desorption/ionization mass spectrometry (MALDI MS) has been used to generate ion images of samples in one or more mass-to-charge (m/z) values, providing the capability of mapping specific molecules to two-dimensional coordinates of the original sample. The high sensitivity of the technique (low-femtomole to attomole levels for proteins and peptides) allows the study of organized biochemical processes occurring in, for example, mammalian tissue sections. The mass spectrometer is used to determine the molecular weights of the molecular in the surface layers of the tissue. Molecules desorbed from the sample typically are singly protonated, giving an ion at (M + H)+, where M is the molecular mass. The procedure involves coating the tissue section, or a blotted imprint of the section, with a thin layer of energy-absorbing matrix and then analyzing the sample to produce an ordered array of mass spectra, each containing nominal m/z values typically covering a range of over 50,000 Da. Images can be displayed in individual m/z values as a selected ion image, which would localize individual compounds in the tissue, or as summed ion images. MALDI ion images of tissue sections can be obtained directly from tissue slices following preparative steps, and this is demonstrated for the mapping of insulin contained in an islet in a section of rat pancreas, hormone peptides in a small area of a section of rat pituitary, and a small protein bound to the membrane of human mucosa cells. Alternatively, imprints of the tissue can be analyzed by blotting the tissue sections on specially prepared targets containing an adsorbent material, e.g., C-18 coated resin beads. Peptides and small proteins bind to the C-18 and create a positive imprint of the tissue which can then be imaged by the mass spectrometer. This is demonstrated for the MALDI ion image analysis of regions of rat splenic pancreas and for an area of rat pituitary traversing the anterior, intermediate, and posterior regions where localized peptides were mapped. In a single spectrum from the anterior/intermediate lobe of a rat pituitary print, over 50 ions corresponding to the peptides present in this tissue were observed as well as precursors, isoforms, and metabolic fragments.
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              The 3D OrbiSIMS—label-free metabolic imaging with subcellular lateral resolution and high mass-resolving power

              Carla F Newman, Peter Marshall, Henrik Arlinghaus … (2017)
              Article 0 comments Cited 124 times – based on 0 reviews     Review now
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                Author and article information

                Contributors
                Kelly Dimovska Nilsson:
                Bio :
                Kelly Dimovska Nilsson

                is a PhD student at the Department of Chemistry and Molecular Biology at the University of Gothenburg, Sweden, working with characterization of new ion sources and implementation of secondary ion mass spectrometry for imaging mass spectrometry of biological samples.

                Anthi Karagianni:
                Bio :
                Anthi Karagianni

                has a degree in chemistry from the Department of Chemistry, University of Patras, Greece, and recently completed a masters in chemistry at the University of Gothenburg, Sweden, specializing in analytical chemistry.

                Ibrahim Kaya:
                Bio :
                Ibrahim Kaya

                is a postdoctoral researcher at the Medical Mass Spectrometry Laboratory, Department of Pharmaceutical Biosciences, Uppsala University, Sweden. He received his PhD from the Department of Psychiatry and Neurochemistry at the Sahlgrenska Academy, University of Gothenburg, Sweden. He has been working on the development and applications of mass spectrometry imaging methods (including SIMS and MALDI) for probing molecular disease pathologies, in particular spatial lipid molecular pathologies in Alzheimer’s and Parkinson’s diseases.

                Marcus Henricsson:
                Bio :
                Marcus Henricsson

                is responsible for the metabolomics facility at the Wallenberg Laboratory at the University of Gothenburg. He has been working for many years in the field of biological mass spectrometry with main focus on biomarker discovery and development in the field of microbiota and cardiometabolic disease.

                John S. Fletcher: john.fletcher@chem.gu.se
                Bio :
                John S. Fletcher

                received his PhD from UMIST (Manchester, UK) in 2004 and is now Professor of Analytical Chemistry at the University of Gothenburg, Sweden. He specializes in imaging mass spectrometry, particularly the development and application of secondary ion mass spectrometry (SIMS) for cell and tissue imaging.

                Journal
                Journal ID (nlm-ta): Anal Bioanal Chem
                Journal ID (iso-abbrev): Anal Bioanal Chem
                Title: Analytical and Bioanalytical Chemistry
                Publisher: Springer Berlin Heidelberg (Berlin/Heidelberg )
                ISSN (Print): 1618-2642
                ISSN (Electronic): 1618-2650
                Publication date (Electronic): 11 May 2021
                Publication date PMC-release: 11 May 2021
                Publication date (Print): 2021
                Volume: 413
                Issue: 16
                Pages: 4181-4194
                Affiliations
                [1 ]GRID grid.8761.8, ISNI 0000 0000 9919 9582, Present Address: Department of Chemistry and Molecular Biology, , University of Gothenburg, ; 405 30 Gothenburg, Sweden
                [2 ]GRID grid.8761.8, ISNI 0000 0000 9919 9582, Department of Psychiatry and Neurochemistry, , Sahlgrenska Academy at the University of Gothenburg, ; 413 45 Mölndal, Sweden
                [3 ]GRID grid.8993.b, ISNI 0000 0004 1936 9457, Medical Mass Spectrometry Laboratory, Department of Pharmaceutical Biosciences, , Uppsala University, ; 751 05 Uppsala, Sweden
                [4 ]GRID grid.8761.8, ISNI 0000 0000 9919 9582, Department of Molecular and Clinical Medicine/Wallenberg Laboratory, Institute of Medicine, , University of Gothenburg, ; 41345 Gothenburg, Sweden
                Author notes

                Published in the topical collection Mass Spectrometry Imaging 2.0 with guest editors Shane R. Ellis and Tiffany Porta Siegel.

                Article
                Publisher ID: 3372
                DOI: 10.1007/s00216-021-03372-x
                PMC ID: 8222020
                PubMed ID: 33974088
                SO-VID: 9141a34e-cd4f-4ee1-b7e5-57899052e88b
                Copyright © © The Author(s) 2021
                License:

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

                History
                Date received : 13 October 2020
                Date revision received : 7 March 2021
                Date accepted : 22 April 2021
                Funding
                Funded by: FundRef http://dx.doi.org/10.13039/501100004359, Vetenskapsrådet;
                Award ID: 2016-04669
                Categories
                Subject: Paper in Forefront
                Custom metadata
                issue-copyright-statement © Springer-Verlag GmbH Germany, part of Springer Nature 2021

                ScienceOpen disciplines: Analytical chemistry
                Keywords: sims,alzheimer’s,lipids,imaging,mass spectrometry,water clusters
                Data availability:
                ScienceOpen disciplines: Analytical chemistry
                Keywords: sims, alzheimer’s, lipids, imaging, mass spectrometry, water clusters

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