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  Cryogenic Infrared Spectroscopy Reveals Structural Modularity in the Vibrational Fingerprints of Heparan Sulfate Diastereomers

Lettow, M., Grabarics, M., Greis, K., Mucha, E., Thomas, D., Chopra, P., et al. (2020). Cryogenic Infrared Spectroscopy Reveals Structural Modularity in the Vibrational Fingerprints of Heparan Sulfate Diastereomers. Analytical Chemistry, 92(15), 10228-10232. doi:10.1021/acs.analchem.0c02048.

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 Creators:
Lettow, Maike1, 2, Author              
Grabarics, Márkó1, 2, Author              
Greis, Kim1, 2, Author              
Mucha, Eike1, Author              
Thomas, Daniel1, Author              
Chopra, Pradeep3, Author
Boons, Geert-Jan3, 4, Author
Karlsson, Richard5, Author
Turnbull, Jeremy E.5, 6, Author
Meijer, Gerard1, Author              
Miller, Rebecca L.2, Author
Helden, Gert von1, Author              
Pagel, Kevin1, 2, Author              
Affiliations:
1Molecular Physics, Fritz Haber Institute, Max Planck Society, ou_634545              
2Institut für Chemie und Biochemie, Freie Universität Berlin, Arnimallee 22, 14195 Berlin, Germany, ou_persistent22              
3Complex Carbohydrate Research Center, University of Georgia, 315 Riverbend Road, Athens, Georgia, United States, ou_persistent22              
4Department of Chemical Biology and Drug Discovery, Utrecht Institute for Pharmaceutical Science, and Bijvoet Center for Biomolecular Research, Utrecht University,, Universiteitsweg 99, 3584 CG Utrecht, The Netherlands, ou_persistent22              
5Copenhagen Centre for Glycomics, Department of Cellular and Molecular Medicine, University of Copenhagen, Copenhagen N 2200, Denmark, ou_persistent22              
6Centre for Glycobiology, Department of Biochemistry, University of Liverpool, Liverpool, L69 7ZB, United Kingdom, ou_persistent22              

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 Abstract: Heparan sulfate and heparin are highly acidic polysaccharides with a linear sequence, consisting of alternating glucosamine and hexuronic acid building blocks. The identity of hexuronic acid units shows a variability along their sequence, as D-glucuronic acid and its C5 epimer, L-iduronic acid can both occur. The resulting backbone diversity represents a major challenge for an unambiguous structural assignment by mass spectrometry-based techniques. Here, we employ cryogenic infrared spectroscopy on mass-selected ions to overcome this challenge and distinguish isomeric heparan sulfate tetrasaccharides that differ only in the configuration of their hexuronic acid building blocks. High-resolution infrared spectra of a systematic set of synthetic heparan sulfate stereoisomers were recorded in the fingerprint region from 1000 to 1800 cm-1 . The experiments reveal a characteristic combination of spectral features for each of the four diastereomers studied, and imply structural modularity in the vibrational fingerprints. Strong spectrum-structure correlations were found and rationalized by state-of-the-art quantum chemical calculations. The findings demonstrate the potential of cryogenic infrared spectroscopy to extend the mass spectrometry-based toolkit for the sequencing of heparan sulfate and structurally related biomolecules. Cited

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Language(s): eng - English
 Dates: 2020-05-122020-07-132020-08-04
 Publication Status: Published in print
 Pages: 5
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.analchem.0c02048
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Title: Analytical Chemistry
  Abbreviation : Anal. Chem.
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: 5 Volume / Issue: 92 (15) Sequence Number: - Start / End Page: 10228 - 10232 Identifier: ISSN: 0003-2700
CoNE: https://pure.mpg.de/cone/journals/resource/111032812862552