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  Molecular dynamics investigation of desorption and ion separation following picosecond infrared laser (PIRL) ablation of an ionic aqueous protein solution

Zou, J., Wu, C., Robertson, W., Zhigilei, L. V., & Miller, R. J. D. (2016). Molecular dynamics investigation of desorption and ion separation following picosecond infrared laser (PIRL) ablation of an ionic aqueous protein solution. The Journal of Chemical Physics, 145(20): 204202. doi:10.1063/1.4967164.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002C-201C-8 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-E0DC-A
Genre: Journal Article

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1.4967164.pdf (Publisher version), 6MB
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© AIP Publishing LLC. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing.

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http://dx.doi.org/10.1063/1.4967164 (Publisher version)
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 Creators:
Zou, J.1, Author
Wu, C.2, Author
Robertson, Wesley3, Author              
Zhigilei, L. V.2, Author
Miller, R. J. Dwayne1, 3, Author              
Affiliations:
1Departments of Chemistry and Physics, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada, ou_persistent22              
2Department of Materials Science and Engineering, University of Virginia, Charlottesville, Virginia 22904-4745, USA, ou_persistent22              
3Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              

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Free keywords: Electric fields; Laser ablation; Bioelectrochemistry; Ion sources; Matrix assisted laser desorption ionization
 Abstract: Molecular dynamics simulations were performed to characterize the ablation process induced by a picosecond infrared laser (PIRL) operating in the regime of desorption by impulsive vibrational excitation (DIVE) of a model peptide (lysozyme)/counter-ion system in aqueous solution. The simulations were performed for ablation under typical experimental conditions found within a time-of-flight mass spectrometer (TOF-MS), that is in vacuum with an applied electric field (E = ± 107 V/m), for up to 2 ns post-ablation and compared to the standard PIRL-DIVE ablation condition (E = 0 V/m). Further, a simulation of ablation under an extreme field condition (E = 1010 V/m) was performed for comparison to extend the effective dynamic range of the effect of the field on charge separation. The results show that the plume dynamics were retained under a typical TOF-MS condition within the first 1 ns of ablation. Efficient desorption was observed with more than 90% of water molecules interacting with lysozyme stripped off within 1 ns post-ablation. The processes of ablation and desolvation of analytes were shown to be independent of the applied electric field and thus decoupled from the ion separation process. Unlike under the extreme field conditions, the electric field inside a typical TOF-MS was shown to modify the ions’ motion over a longer time and in a soft manner with no enhancement to fragmentation observed as compared to the standard PIRL-DIVE. The study indicates that the PIRL-DIVE ablation mechanism could be used as a new, intrinsically versatile, and highly sensitive ion source for quantitative mass spectrometry.

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Language(s): eng - English
 Dates: 2016-07-182016-10-032016-11-302016-11-28
 Publication Status: Published in print
 Pages: 12
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1063/1.4967164
 Degree: -

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Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: - Volume / Issue: 145 (20) Sequence Number: 204202 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: /journals/resource/954922836226