% IMPORTANT: The following is UTF-8 encoded. This means that in the presence % of non-ASCII characters, it will not work with BibTeX 0.99 or older. % Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or % “biber”. @ARTICLE{Li:829373, author = {Li, Jinyu and Lyu, Wenping and Rossetti, Giulia and Konijnenberg, Albert and Natalello, Antonino and Ippoliti, Emiliano and Orozco, Modesto and Sobott, Frank and Grandori, Rita and Carloni, Paolo}, title = {{P}roton {D}ynamics in {P}rotein {M}ass {S}pectrometry}, journal = {The journal of physical chemistry letters}, volume = {8}, number = {6}, issn = {1948-7185}, address = {Washington, DC}, publisher = {ACS}, reportid = {FZJ-2017-03086}, pages = {1105 - 1112}, year = {2017}, abstract = {Native electrospray ionization/ion mobility-mass spectrometry (ESI/IM-MS) allows an accurate determination of low-resolution structural features of proteins. Yet, the presence of proton dynamics, observed already by us for DNA in the gas phase, and its impact on protein structural determinants, have not been investigated so far. Here, we address this issue by a multistep simulation strategy on a pharmacologically relevant peptide, the N-terminal residues of amyloid-β peptide (Aβ(1–16)). Our calculations reproduce the experimental maximum charge state from ESI-MS and are also in fair agreement with collision cross section (CCS) data measured here by ESI/IM-MS. Although the main structural features are preserved, subtle conformational changes do take place in the first ∼0.1 ms of dynamics. In addition, intramolecular proton dynamics processes occur on the picosecond-time scale in the gas phase as emerging from quantum mechanics/molecular mechanics (QM/MM) simulations at the B3LYP level of theory. We conclude that proton transfer phenomena do occur frequently during fly time in ESI-MS experiments (typically on the millisecond time scale). However, the structural changes associated with the process do not significantly affect the structural determinants.}, cin = {IAS-5 / INM-9 / JSC}, ddc = {530}, cid = {I:(DE-Juel1)IAS-5-20120330 / I:(DE-Juel1)INM-9-20140121 / I:(DE-Juel1)JSC-20090406}, pnm = {574 - Theory, modelling and simulation (POF3-574) / 511 - Computational Science and Mathematical Methods (POF3-511)}, pid = {G:(DE-HGF)POF3-574 / G:(DE-HGF)POF3-511}, typ = {PUB:(DE-HGF)16}, UT = {WOS:000396975600001}, pubmed = {pmid:28207277}, doi = {10.1021/acs.jpclett.7b00127}, url = {https://juser.fz-juelich.de/record/829373}, }