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Fragmentation of Neutral Amino Acids and Small Peptides by Intense, Femtosecond Laser Pulses

  • Martin J. Duffy
    Martin J. Duffy
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
  • Orla Kelly
    Orla Kelly
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
    More by Orla Kelly
  • Christopher R. Calvert
    Christopher R. Calvert
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
  • Raymond B. King
    Raymond B. King
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
  • Louise Belshaw
    Louise Belshaw
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
  • Thomas J. Kelly
    Thomas J. Kelly
    National Centre for Plasma Science and Technology, School of Physical Sciences, Dublin City University, Dublin, Republic of Ireland
  • John T. Costello
    John T. Costello
    National Centre for Plasma Science and Technology, School of Physical Sciences, Dublin City University, Dublin, Republic of Ireland
  • David J. Timson
    David J. Timson
    School of Biological Sciences, Queen’s University Belfast, BT9 7BL, Belfast, UK
  • William A. Bryan
    William A. Bryan
    Department of Physics, Swansea University, SA2 8PP, Swansea, UK
  • Thomas Kierspel
    Thomas Kierspel
    STFC Rutherford Appleton Laboratory, OX11 0QX, Didcot, Oxon, UK
    Center for Free‐Electron Laser Science, DESY, Notkestrasse 85, 22607, Hamburg, Germany
  • I. C. Edmond Turcu
    I. C. Edmond Turcu
    STFC Rutherford Appleton Laboratory, OX11 0QX, Didcot, Oxon, UK
  • Cephise M. Cacho
    Cephise M. Cacho
    STFC Rutherford Appleton Laboratory, OX11 0QX, Didcot, Oxon, UK
  • Emma Springate
    Emma Springate
    STFC Rutherford Appleton Laboratory, OX11 0QX, Didcot, Oxon, UK
  • Ian D. Williams
    Ian D. Williams
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
  • , and 
  • Jason B. Greenwood
    Jason B. Greenwood
    Centre for Plasma Physics, School of Mathematics and Physics, Queen’s University Belfast, BT7 1NN, Belfast, UK
Cite this: J. Am. Soc. Mass Spectrom. 2013, 24, 9, 1366–1375
Publication Date (Web):July 2, 2013
https://doi.org/10.1007/s13361-013-0653-6
Copyright © 2013 © American Society for Mass Spectrometry 2013

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    Abstract

    Abstract Image

    High power femtosecond laser pulses have unique properties that could lead to their application as ionization or activation sources in mass spectrometry. By concentrating many photons into pulse lengths approaching the timescales associated with atomic motion, very strong electric field strengths are generated, which can efficiently ionize and fragment molecules without the need for resonant absorption. However, the complex interaction between these pulses and biomolecular species is not well understood. To address this issue, we have studied the interaction of intense, femtosecond pulses with a number of amino acids and small peptides. Unlike previous studies, we have used neutral forms of these molecular targets, which allowed us to investigate dissociation of radical cations without the spectra being complicated by the action of mobile protons. We found fragmentation was dominated by fast, radical-initiated dissociation close to the charge site generated by the initial ionization or from subsequent ultrafast migration of this charge. Fragments with lower yields, which are useful for structural determinations, were also observed and attributed to radical migration caused by hydrogen atom transfer within the molecule.

    Cited By

    This article is cited by 9 publications.

    1. Andrey Krutilin, Sascha W. Epp, Glaynel M. L. Alejo, Frederik Busse, Djordje Gitaric, Hendrik Schikora, Heinrich Schwoerer, Friedjof Tellkamp. Peptide Mass Spectra from Micrometer-Thick Ice Films Produced with Femtosecond Pulses. Analytical Chemistry 2022, 94 (39) , 13359-13367. https://doi.org/10.1021/acs.analchem.2c01810
    2. Tatsuro Shirota, Masashi Tsuge, Yasumasa Hikosaka, Koichi Soejima, and Kennosuke Hoshina . Detection of Neutral Species in the MALDI Plume Using Femtosecond Laser Ionization: Quantitative Analysis of MALDI-MS Signals Based on a Semiequilibrium Proton Transfer Model. The Journal of Physical Chemistry A 2017, 121 (1) , 31-39. https://doi.org/10.1021/acs.jpca.6b09591
    3. Jason B. Greenwood, Jordan Miles, Simone De Camillis, Peter Mulholland, Lijuan Zhang, Michael A. Parkes, Helen C. Hailes, and Helen H. Fielding . Resonantly Enhanced Multiphoton Ionization Spectrum of the Neutral Green Fluorescent Protein Chromophore. The Journal of Physical Chemistry Letters 2014, 5 (20) , 3588-3592. https://doi.org/10.1021/jz5019256
    4. Cornelius L. Pieterse, Jason M. Gross, Luke Hanley. Ultrashort Pulse Photoionization for Femtosecond Laser Mass Spectrometry. 2021, 245-265. https://doi.org/10.1002/9783527682201.ch7
    5. Rebecca Meißner, Linda Feketeová, Andreas Bayer, Johannes Postler, Paulo Limão-Vieira, Stephan Denifl. Positive and negative ions of the amino acid histidine formed in low-energy electron collisions. Journal of Mass Spectrometry 2019, 54 (10) , 802-816. https://doi.org/10.1002/jms.4427
    6. Francesca Calegari, Andrea Trabattoni, Alicia Palacios, David Ayuso, Mattea C Castrovilli, Jason B Greenwood, Piero Decleva, Fernando Martín, Mauro Nisoli. Charge migration induced by attosecond pulses in bio-relevant molecules. Journal of Physics B: Atomic, Molecular and Optical Physics 2016, 49 (14) , 142001. https://doi.org/10.1088/0953-4075/49/14/142001
    7. Mohammad M Rafiee Fanood, N. Bhargava Ram, C. Stefan Lehmann, Ivan Powis, Maurice H. M. Janssen. Enantiomer-specific analysis of multi-component mixtures by correlated electron imaging–ion mass spectrometry. Nature Communications 2015, 6 (1) https://doi.org/10.1038/ncomms8511
    8. Geert Reitsma, Olmo Gonzalez-Magaña, Oscar Versolato, Meike Door, Ronnie Hoekstra, Eric Suraud, Bettina Fischer, Nicolas Camus, Manuel Kremer, Robert Moshammer, Thomas Schlathölter. Femtosecond laser induced ionization and dissociation of gas-phase protonated leucine enkephalin. International Journal of Mass Spectrometry 2014, 365-366 , 365-371. https://doi.org/10.1016/j.ijms.2014.01.004
    9. James N. Bull, Jason W.L. Lee, Sara H. Gardiner, Claire Vallance. Account: An Introduction to Velocity-Map Imaging Mass Spectrometry (VMImMS). European Journal of Mass Spectrometry 2014, 20 (2) , 117-129. https://doi.org/10.1255/ejms.1264

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