Skip to main content

Activation and Dissociation of Large Molecules in Mass Spectrometry


EMSL Project ID
24493

Abstract

This proposal is a continuation of research under EMSL User Proposal #6291. Mass spectrometry is unique among instrumental analysis techniques in terms of its extraordinary sensitivity, molecular specificity and utility for addressing key questions in a broad range of scientific disciplines. The purpose of our research is to achieve a fundamental understanding of the kinetics and dynamics of activating and dissociating complex molecular ions. These processes are the scientific foundation for tandem mass spectrometry, one of the most important analytical methods developed in the last century. Because of their large number of internal degrees of freedom the kinetics of dissociation of large molecular ions are qualitatively and quantitatively different from the analogous behaviour of small molecule counterparts. This makes the study of complex systems interesting from both a fundamental and applied (analytical mass spectrometry) perspective. We have utilized surface-induced dissociation (SID) as a means for depositing very rapidly (a few hundred femtoseconds) relatively large and controllable amounts of internal energy in protonated model peptides as a technically important class of complex molecules, whose characteri-zation by tandem mass spectrometry is central to the emerging field of proteomics.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2007-06-01
End Date
2010-09-30
Status
Closed

Team

Principal Investigator

Julia Laskin
Institution
Purdue University

Team Members

Patrick Roach
Institution
Pacific Northwest National Laboratory

Grant Johnson
Institution
Pacific Northwest National Laboratory

Qichi Hu
Institution
Pacific Northwest National Laboratory

Jeffrey Smith
Institution
University of Washington

Zhibo Yang
Institution
University of Colorado at Boulder

Related Publications

Bateman AP, ML Walser, Y Dessiaterik, J Laskin, A Laskin, and S Nizkorodov.  2008.  "The Effect of Solvent on the Analysis of Secondary Organic Aerosol Using Electrospray Ionization Mass Spectrometry."  Environmental Science & Technology 42(19):7341-7346.  doi:10.1021/es801226w
Chang-Graham AL, LT Profeta, TJ Johnson, RJ Yokelson, A Laskin, and J Laskin. 2011. "Case Study of Water-Soluble Metal Containing Organic Constituents of Biomass Burning Aerosol." Environmental Science & Technology 45(4):1257-1263. doi:10.1021/es103010j
Laskin A, JS Smith, and J Laskin. 2009. "Molecular Characterization of Nitrogen Containing Organic Compounds in Biomass Burning Aerosols Using High Resolution Mass Spectrometry." Environmental Science & Technology 43(10):3764-3771. doi:10.1021/es803456n
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
Ng DC, T Song, SO Siu, CK Siu, J Laskin, and IK Chu. 2010. "Formation, isomerization, and dissociation of alpha-carbon-centered and pi-centered glycylglycyltryptophan radical cations." Journal of Physical Chemistry B 114(6):2270-2280. doi:10.1021/jp908599a
Roach PJ, J Laskin, and A Laskin. 2010. "Nanospray Desorption Electrospray Ionization: an Ambient Method for Liquid-Extraction Surface Sampling in Mass Spectrometry." Analyst 135(9):2233-2236.
Smith JS, A Laskin, and J Laskin. 2009. "Molecular Characterization of Biomass Burning Aerosols Using High Resolution Mass Spectrometry." Analytical Chemistry 81(4):1512-1521. doi:10.1021/ac8020664
Spraggins JM, JA Lloyd, MV Johnston, J Laskin, and DP Ridge.  2009.  "Fragmentation Mechanisms of Oxidized Peptides Elucidated by SID, RRKM Modeling and Molecular Dynamics."  Journal of the American Society for Mass Spectrometry 20(9):1579-1592.  doi:10.1016/j.jasms.2009.04.012
Yang Z, C Lam, IK Chu, and J Laskin. 2008. "The Effect of the Secondary Structure on Dissociation of Peptide Radical Cations: Fragmentation of Angiotensin III and Its Analogues." Journal of Physical Chemistry B 112(39):12468-12478. doi:10.1021/jp805226x
Yang Z, ER Vorpagel, and J Laskin.  2008.  "Experimental and Theoretical Studies of the Structures and Interactions of Vancomycin Antibiotics with Cell Wall Analogues."  Journal of the American Chemical Society 130(39):13013-13022.  doi:10.1021/ja802643g.
Yang Z, ER Vorpagel, and J Laskin. 2009. "Influence of the Charge State on the Structures and Interactions of Vancomycin Antibiotics with Cell-Wall Analogue Peptides: Experimental and Theoretical Studies." Chemistry - a European Journal 15(9):2081-2090. doi:10.1002/chem.200802010.
Z. Yang, O. Hadjar and J. Laskin. “Effect of the Surface Morphology on the Energy Transfer in Ion-Surface Collisions,” Int. J. Mass Spectrom., Jean Futrell Honor Issue, 265, 124–129 (2007).