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Title: Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers

Abstract

Structural isomers, molecules having the same chemical formula but with atoms bonded in different order, are hard to identify using conventional spectroscopy and mass spectrometry. They exhibit virtually indistinguishable mass spectra when ionized by electrons. Laser mass spectrometry based on photoionization of the isomers has emerged as a promising alternative but requires shaped ultrafast laser pulses. Here we use transform limited femtosecond pulses to distinguish the isomers using two methods. First, we probe doubly charged parent ions with circularly polarized light. We show that the yield of doubly charged ortho-xylene decreases while para-xylene increases over a range of laser intensities when the laser polarization is changed from linear to circular. Second, we probe high harmonic generation from randomly oriented isomer molecules subjected to an intense laser field. Here we show that the yield of high-order harmonics varies with the positioning of the methyl group in xylene isomers (ortho-, para- and meta-) and is due to differences in the strength of tunnel ionization and the overlap between the angular peaks of ionization and photo-recombination.

Authors:
 [1];  [2];  [3];  [4];  [3];  [3];  [3]; ORCiD logo [3];  [5];  [4]; ORCiD logo [4];  [3]; ORCiD logo [6];  [2]
+ Show Author Affiliations
  1. Univ. of Ottawa, Ottawa, ON (Canada); King Abdulaziz City for Science and Technology (KACST), Riyadh (Saudi Arabia)
  2. Univ. of Ottawa, Ottawa, ON (Canada)
  3. Imperial College London, London (United Kingdom)
  4. INRS-EMT, Varennes (Canada)
  5. Instituto de Química Fisica Rocasolano, Madrid (Spain)
  6. Kansas State Univ., Manhattan, KS (United States)
Publication Date:
Research Org.:
Kansas State Univ., Manhattan, KS (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1500098
Grant/Contract Number:  
FG02-86ER13491
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Alharbi, Abdullah, Boguslavskiy, Andrey E., Austin, Dane, Thiré, Nicolas, Wood, D., Hawkins, P., McGrath, Felicity, Johnson, A. S., Lopez-Quintas, I., Schmidt, Bruno, Légaré, Francois, Marangos, J. P., Le, Anh -Thu, and Bhardwaj, Ravi. Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers. United States: N. p., 2018. Web. doi:10.1038/s41598-018-22055-9.
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Alharbi, Abdullah, Boguslavskiy, Andrey E., Austin, Dane, Thiré, Nicolas, Wood, D., Hawkins, P., McGrath, Felicity, Johnson, A. S., Lopez-Quintas, I., Schmidt, Bruno, Légaré, Francois, Marangos, J. P., Le, Anh -Thu, & Bhardwaj, Ravi. Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers. United States. doi:10.1038/s41598-018-22055-9.
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Alharbi, Abdullah, Boguslavskiy, Andrey E., Austin, Dane, Thiré, Nicolas, Wood, D., Hawkins, P., McGrath, Felicity, Johnson, A. S., Lopez-Quintas, I., Schmidt, Bruno, Légaré, Francois, Marangos, J. P., Le, Anh -Thu, and Bhardwaj, Ravi. Wed . "Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers". United States. doi:10.1038/s41598-018-22055-9. https://www.osti.gov/servlets/purl/1500098.
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@article{osti_1500098,
title = {Femtosecond Laser Mass Spectrometry and High Harmonic Spectroscopy of Xylene Isomers},
author = {Alharbi, Abdullah and Boguslavskiy, Andrey E. and Austin, Dane and Thiré, Nicolas and Wood, D. and Hawkins, P. and McGrath, Felicity and Johnson, A. S. and Lopez-Quintas, I. and Schmidt, Bruno and Légaré, Francois and Marangos, J. P. and Le, Anh -Thu and Bhardwaj, Ravi},
abstractNote = {Structural isomers, molecules having the same chemical formula but with atoms bonded in different order, are hard to identify using conventional spectroscopy and mass spectrometry. They exhibit virtually indistinguishable mass spectra when ionized by electrons. Laser mass spectrometry based on photoionization of the isomers has emerged as a promising alternative but requires shaped ultrafast laser pulses. Here we use transform limited femtosecond pulses to distinguish the isomers using two methods. First, we probe doubly charged parent ions with circularly polarized light. We show that the yield of doubly charged ortho-xylene decreases while para-xylene increases over a range of laser intensities when the laser polarization is changed from linear to circular. Second, we probe high harmonic generation from randomly oriented isomer molecules subjected to an intense laser field. Here we show that the yield of high-order harmonics varies with the positioning of the methyl group in xylene isomers (ortho-, para- and meta-) and is due to differences in the strength of tunnel ionization and the overlap between the angular peaks of ionization and photo-recombination.},
doi = {10.1038/s41598-018-22055-9},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {2018},
month = {2}
}
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Journal Article:
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DOI:  10.1038/s41598-018-22055-9
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Figures / Tables:

Figure 1 Figure 1: Femtosecond laser mass spectrum of o- and p-xylene. (a) Time-of-flight mass spectrum of o-xylene at 800 nm and laser intensity of 1014/W/cm2. The inset shows the structure of the three xylene isomers. (b,c) Portion of the mass spectrum containing the signal of doubly charged ions of p-xylene (red)more » and o-xylene (blue) for linear polarization and, (c) for circular polarization. Only the portion of spectra containing the signals of doubly charged ions are shown. (d) The ratio of doubly charged p-xylene signal at m/q = 53 to that of o-xylene at 800 nm for linear polarization (blue squares) and circular polarization (black circles). Also is shown the same ratio for the isotope signal at m/q = 53.5 for circularly polarized light (red diamonds). The doubly charged signal was normalized to the parent ion.« less
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    Works referencing / citing this record:

    Real-Time Distinguishing of the Xylene Isomers Using Photoionization and Dissociation Mass Spectra Obtained by Femtosecond Laser Mass Spectrometry (FLMS)
    journal, July 2019

    • Kepceoğlu, Abdullah; Gündoğdu, Yasemin; Ledingham, Kenneth William David
    • Analytical Letters, Vol. 53, Issue 2
    • DOI: 10.1080/00032719.2019.1647227
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