skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Comprehensive Peptide Ion Structure Studies Using Ion Mobility Techniques: Part 3. Relating Solution-Phase to Gas-Phase Structures

Abstract

Molecular dynamics (MD) simulations have been utilized to study peptide ion conformer establishment during the electrospray process. An explicit water model is used for nanodroplets containing a model peptide and hydronium ions. Simulations are conducted at 300 K for two different peptide ion charge configurations and for droplets containing varying numbers of hydronium ions. For all conditions, modeling has been performed until production of the gas-phase ions and the resultant conformers have been compared to proposed gas-phase structures. The latter species were obtained from previous studies in which in silico candidate structures were filtered according to ion mobility and hydrogen-deuterium exchange (HDX) reactivity matches. Results from the present study present three key findings namely (1) the evidence from ion production modeling supports previous structure refinement studies based on mobility and HDX reactivity matching, (2) the modeling of the electrospray process is significantly improved by utilizing initial droplets existing below but close to the calculated Rayleigh limit, and (3) peptide ions in the nanodroplets sample significantly different conformers than those in the bulk solution due to altered physicochemical properties of the solvent. .

Authors:
;  [1];  [2]
  1. Johns Hopkins University, Department of Biophysics (United States)
  2. West Virginia University, Department of Chemistry (United States)
Publication Date:
OSTI Identifier:
22776865
Resource Type:
Journal Article
Journal Name:
Journal of the American Society for Mass Spectrometry
Additional Journal Information:
Journal Volume: 29; Journal Issue: 8; Other Information: Copyright (c) 2018 American Society for Mass Spectrometry; http://www.springer-ny.com; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 1044-0305
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; COMPARATIVE EVALUATIONS; DEUTERIUM; HYDROGEN; ION MOBILITY; IONIZATION; MOLECULAR DYNAMICS METHOD; OXONIUM IONS; PEPTIDES; SIMULATION; SOLUTIONS

Citation Formats

Kondalaji, Samaneh Ghassabi, Khakinejad, Mahdiar, and Valentine, Stephen J., E-mail: stephen.valentine@mail.wvu.edu. Comprehensive Peptide Ion Structure Studies Using Ion Mobility Techniques: Part 3. Relating Solution-Phase to Gas-Phase Structures. United States: N. p., 2018. Web. doi:10.1007/S13361-018-1996-9.
Kondalaji, Samaneh Ghassabi, Khakinejad, Mahdiar, & Valentine, Stephen J., E-mail: stephen.valentine@mail.wvu.edu. Comprehensive Peptide Ion Structure Studies Using Ion Mobility Techniques: Part 3. Relating Solution-Phase to Gas-Phase Structures. United States. doi:10.1007/S13361-018-1996-9.
Kondalaji, Samaneh Ghassabi, Khakinejad, Mahdiar, and Valentine, Stephen J., E-mail: stephen.valentine@mail.wvu.edu. Wed . "Comprehensive Peptide Ion Structure Studies Using Ion Mobility Techniques: Part 3. Relating Solution-Phase to Gas-Phase Structures". United States. doi:10.1007/S13361-018-1996-9.
@article{osti_22776865,
title = {Comprehensive Peptide Ion Structure Studies Using Ion Mobility Techniques: Part 3. Relating Solution-Phase to Gas-Phase Structures},
author = {Kondalaji, Samaneh Ghassabi and Khakinejad, Mahdiar and Valentine, Stephen J., E-mail: stephen.valentine@mail.wvu.edu},
abstractNote = {Molecular dynamics (MD) simulations have been utilized to study peptide ion conformer establishment during the electrospray process. An explicit water model is used for nanodroplets containing a model peptide and hydronium ions. Simulations are conducted at 300 K for two different peptide ion charge configurations and for droplets containing varying numbers of hydronium ions. For all conditions, modeling has been performed until production of the gas-phase ions and the resultant conformers have been compared to proposed gas-phase structures. The latter species were obtained from previous studies in which in silico candidate structures were filtered according to ion mobility and hydrogen-deuterium exchange (HDX) reactivity matches. Results from the present study present three key findings namely (1) the evidence from ion production modeling supports previous structure refinement studies based on mobility and HDX reactivity matching, (2) the modeling of the electrospray process is significantly improved by utilizing initial droplets existing below but close to the calculated Rayleigh limit, and (3) peptide ions in the nanodroplets sample significantly different conformers than those in the bulk solution due to altered physicochemical properties of the solvent. .},
doi = {10.1007/S13361-018-1996-9},
journal = {Journal of the American Society for Mass Spectrometry},
issn = {1044-0305},
number = 8,
volume = 29,
place = {United States},
year = {2018},
month = {8}
}