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Electron capture induced dissociation of doubly protonated pentapeptides: Dependence on molecular structure and charge separation
Stockholms universitet, Naturvetenskapliga fakulteten, Fysikum.
Stockholms universitet, Naturvetenskapliga fakulteten, Fysikum.
Stockholms universitet, Naturvetenskapliga fakulteten, Fysikum.
Stockholms universitet, Naturvetenskapliga fakulteten, Fysikum.ORCID-id: 0000-0002-2493-4161
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2011 (Engelska)Ingår i: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 134, nr 3, s. 035102-Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We have studied electron capture induced dissociation of a set of doubly protonated pentapeptides, all composed of one lysine (K) and either four glycine (G) or four alanine (A) residues, as a function of the sequence of these building blocks. Thereby the separation of the two charges, sequestered on the N-terminal amino group and the lysine side chain, is varied. The characteristic cleavage of N–Cα bonds is observed for all peptides over the whole backbone length, with the charge carrying fragments always containing K. The resulting fragmentation patterns are very similar if G is replaced by A. In the case of [XKXXX+2H]2+ (X=A or G), a distinct feature is observed in the distribution of backbone cleavage fragments and the probability for ammonia loss is drastically reduced. This may be due to an isomer with an amide oxygen as protonation site giving rise to the observed increase in breakage at a specific site in the molecule. For the other peptides, a correlation with the distance between amide oxygen and the charge at the lysine side chain has been found. This may be an indication that it is only the contribution from this site to the charge stabilization of the amide π* orbitals which determines relative fragment intensities. For comparison, complexes with two crown ether molecules have been studied as well. The crown ether provides a shielding of the charge and prevents the peptide from folding and internal hydrogen bonding, which leads to a more uniform fragmentation behavior.

Ort, förlag, år, upplaga, sidor
2011. Vol. 134, nr 3, s. 035102-
Nationell ämneskategori
Fysik
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fysik
Identifikatorer
URN: urn:nbn:se:su:diva-54521DOI: 10.1063/1.3533952ISI: 000286472200071OAI: oai:DiVA.org:su-54521DiVA, id: diva2:395190
Tillgänglig från: 2011-02-04 Skapad: 2011-02-04 Senast uppdaterad: 2019-12-04Bibliografiskt granskad
Ingår i avhandling
1. Probing biomolecular fragmentation
Öppna denna publikation i ny flik eller fönster >>Probing biomolecular fragmentation
2011 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

This thesis deals with fragmentation of complex molecular ions, especially biomolecules, in gas phase collision experiments. The aim is to investigate the relations between energy deposition and fragmentation and to shed light on the mechanisms behind energy and charge transfer processes in collisions involving the building blocks of life. Further, the question how a solvent environment influences the dissociation behavior is elucidated. In the first part of the thesis, results from different collision experiments with biomolecular ions are presented, focusing on electron capture induced dissociation of hydrated nucleotides and small peptides. The investigated processes may be relevant for the understanding of radiation damage and the optimization of sequencing methods used in protein research. Our results clearly demonstrate that effects due to surrounding solvent molecules are substantial. While the dissipation of internal energy by evaporation of the loosely bound solvent molecules may protect the biomolecule, the influence which this environment has on the electronic structure may lead to an enhancement or suppression of certain dissociation channels. The second part of the thesis focuses on recent instrumental developments. Here, the aim was to optimize and complement the techniques used in the experiments above and to have versatile tools available for different kinds of gas phase collision studies involving complex molecular ions. Therefore, we have constructed an electrospray ion source platform for the preparation of intense beams, with options of accumulation and cooling of mass selected ions, allowing for a large variety of experiments. This device is also intended to serve as an ion source for the new storage ring facility DESIREE (DoubleElectroStatic Ion Ring ExpEriment), which is currently under construction at Stockholm University. In these unique storage rings, oppositely charged ions may interact at very low relative velocities in a cryogenically cooled and ultrahigh vacuum environment.

Ort, förlag, år, upplaga, sidor
Stockholm: Department of Physics, Stockholm University, 2011. s. 124
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Fysik
Forskningsämne
fysik
Identifikatorer
urn:nbn:se:su:diva-54524 (URN)978-91-7447-228-8 (ISBN)
Disputation
2011-03-11, FB55, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 13:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2011-02-17 Skapad: 2011-02-04 Senast uppdaterad: 2011-02-07Bibliografiskt granskad

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Haag, NicoleHolm, Anne I. S.Johansson, Henrik A. B.Zettergren, HenningSchmidt, Henning T.Cederquist, Henrik
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