Determining the Gas-Phase Structures of α-Helical Peptides: Insights from Shape, Intramolecular Distance, and Microsolvation Assays

Autor: Wu, Ri, Metternich, Jonas B., Kamenik, Anna S., Tiwari, Prince, Harrison, Julian A., Kessen, Dennis, Akay, Hasan, Benzenberg, Lukas R., Chan, T.‐W. Dominic, Riniker, Sereina, Zenobi, Renato
Jazyk: angličtina
Rok vydání: 2023
Zdroj: Nature Communications
ISSN: 2041-1723
Popis: Mass spectrometry is a powerful technique for the structural and functional characterization of biomolecules. However, it remains challenging to accurately probe the gas-phase structure of biomolecular ions. In this work, we propose a new, synergistic approach which utilizes ion mobility-mass spectrometry, Förster resonance energy transfer, and differential ion mobility spectrometry to provide multiple constraints for molecular modelling of gasphase ion structures. This combined strategy showed superb capabilities for distinguishing conformers and was employed to understand the gas-phase structures of two isomeric α-helical peptides that might differ in helicity. Shape and intramolecular distance constraints were included in structure-refinement calculations after an extensive conformational search. We added microsolvation calculations to assess the interaction sites and energies between the peptide ions and the gaseous additives, which confirmed differences in experimentally observed differential mobilities. Our work allows more rigorous and comprehensive structural characterization of biomolecular ions in the gas phase.
Nature Communications
ISSN:2041-1723
Databáze: OpenAIRE
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