Surface-Induced Dissociation of Large Molecules in Mass Spectrometry
EMSL Project ID
39717
Abstract
The general objective of our research is to achieve a fundamental understanding of the reaction kinetics and dynamics of activating and dissociating complex molecular ions, develop molecular level understanding of interactions of complex ions and molecules with surfaces, and develop new approaches for selective modification of substrates using beams of mass-selected hyperthermal ions. Our research addresses analytical challenges relevant to a broad range of applications within the Department of Energy (DOE) mission areas. Understanding ion activation and dissociation provides the scientific foundation for tandem mass spectrometry, one of the most important analytical methods developed in the last century. We investigate collisional activation and dissociation of a variety of complex molecules including protonated and deprotonated peptides, peptide radical cations and anions, non-covalent complexes, and metalloorganic complexes. Characterization of these molecules using tandem mass spectrometry is central to several fields including proteomics and catalysis, and is essential for understanding self assembly and molecular recognition processes. Our findings obtained for these model systems are relevant to a broader class of complex molecules in biofuels, petroleum samples, and constituents of secondary organic aerosols that are of specific interest to DOE. We investigate the dynamics of surface-induced dissociation (SID) of large molecules and the influence of physical and chemical properties of SID targets on the energy transfer into complex ions using time- and collision energy-resolved measurements in FT-ICR MS. Theoretical modeling of experimental data provides information on the energetics and dynamics of complex ion dissociation processes. EMSL provides unique resources necessary for the proposed research.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2010-10-01
End Date
2013-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Bzdek BR, JW Depalma, DP Ridge, J Laskin, and MV Johnston. 2013. "Fragmentation Energetics of Clusters Relevant to Atmospheric New Particle Formation." Journal of the American Chemical Society 135(8):3276-3285. doi:10.1021/ja3124509
Eckert PA, PJ Roach, A Laskin, and J Laskin. 2012. "Chemical Characterization of Crude Petroleum Using Nanospray Desorption Electrospray Ionization Coupled with High-Resolution Mass Spectrometry." Analytical Chemistry 84(3):1517-1525. doi:10.1021/ac202801g
Hu Q, and J Laskin. 2014. "Reactive Landing of Dendrimer Ions onto Activated Self-assembled Monolayer Surfaces." Physical Chemistry Chemical Physics. PCCP. doi:10.1021/jp411637w
Johnson GE, NM Al Hasan, and J Laskin. 2013. "Influence of Heteroanion and Ammonium Cation Size on the Composition and Gas-Phase Fragmentation of Polyoxovanadates." International Journal of Mass Spectrometry 354-355:333-341. doi:10.1016/j.ijms.2013.06.009
Laskin J, A Laskin, and S Nizkorodov. 2013. "New Mass Spectrometry Techniques for Studying Physical Chemistry of Atmospheric Heterogeneous Processes." International Reviews in Physical Chemistry 32(1):128-170. doi:10.1080/0144235X.2012.752904
Laskin J, and JH Futrell. "New approach for studying slow fragmentation kinetics in FT-ICR: Surface-induced dissociation combined with resonant ejection." International Journal of Mass Spectrometry. doi:10.1016/j.ijms.2014.07.029
Laskin J, and P Wang. 2014. "Charge Retention by Organometallic Dications on Self-Assembled Monolayer Surfaces." International Journal of Mass Spectrometry. doi:10.1016/j.ijms.2014.01.012
Laskin J, and Q Hu. 2017. "Reactive Landing of Gramicidin S and Ubiquitin Ions onto Activated Self-Assembled Monolayer Surfaces." Journal of the American Society for Mass Spectrometry 28(7):1304-1312. doi:10.1007/s13361-017-1614-2
Laskin J, and Z Yang. 2011. "Energetics and Dynamics of Dissociation of Deprotonated Peptides: Fragmentation of Angiotensin Analogs." International Journal of Mass Spectrometry 308(2-3):275-280. doi:10.1016/j.ijms.2011.07.003
Laskin J, BS Heath, PJ Roach, LH Cazares, and OJ Semmes. 2012. "Tissue Imaging Using Nanospray Desorption Electrospray Ionization Mass Spectrometry." Analytical Chemistry 84(1):141-148. doi:10.1021/ac2021322
Laskin J. "Ion–surface collisions in mass spectrometry: Where analytical chemistry meets surface science." International Journal of Mass Spectrometry. doi:10.1016/j.ijms.2014.07.004
Laskin J, PA Eckert, PJ Roach, BS Heath, SA Nizkorodov, and A Laskin. 2012. "Chemical Analysis of Complex Organic Mixtures Using Reactive Nanospray Desorption Electrospray Ionization Mass Spectrometry." Analytical Chemistry 84(16):7179-7187. doi:10.1021/ac301533z
Laskin J, Z Yang, and AS Woods. 2011. "Competition between Covalent and Noncovalent Bond Cleavages in Dissociation of Phosphopeptide-Amine Complexes." Physical Chemistry Chemical Physics. PCCP 13(15):6936-6946. doi:10.1039/C1CP00029B
Laskin J, Z Yang, T Song, C Lam, and IK Chu. 2010. "Effect of the Basic Residue on the Energetics, Dynamics and Mechanisms of Gas- Phase Fragmentation of Protonated Peptides." Journal of the American Chemical Society 132(45):16006-16016. doi:10.1021/ja104438z
Lin P, J Liu, JE Shilling, SM Kathmann, J Laskin, and A Laskin. 2015. "Molecular characterization of brown carbon (BrC) chromophores in secondary organic aerosol generated from photo-oxidation of toluene." Physical Chemistry Chemical Physics. doi:10.1039/C5CP02563J
Olivares AM, J Laskin, and GE Johnson. 2014. "Investigating the Synthesis of Ligated Metal Clusters in Solution Using a Flow Reactor and Electrospray Ionization Mass Spectrometry." Journal of Physical Chemistry A.
Roach PJ, J Laskin, and A Laskin. 2011. "Higher-Order Mass Defect Analysis for Mass Spectra of Complex Organic Mixtures." Analytical Chemistry 83(12):4924-4929. doi:10.1021/ac200654j
Zhang W, D Du, KDD Gunaratne, RJ Colby, Y Lin, and J Laskin. 2013. "Polyoxometalate-Graphene Nanocomposite Modified Electrode for Electrocatalytic Detection of Ascorbic Acid." Electrochemistry Communications 26(1):178-183. doi:10.1002/elan.201300343