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Title: Mechanisms and time-resolved dynamics for trihydrogen cation (H 3 +) formation from organic molecules in strong laser fields

Strong-field laser-matter interactions often lead to exotic chemical reactions. Trihydrogen cation formation from organic molecules is one such case that requires multiple bonds to break and form. Here, we present evidence for the existence of two different reaction pathways for H 3 + formation from organic molecules irradiated by a strong-field laser. Assignment of the two pathways was accomplished through analysis of femtosecond time-resolved strong-field ionization and photoion-photoion coincidence measurements carried out on methanol isotopomers, ethylene glycol, and acetone. Ab initio molecular dynamics simulations suggest the formation occurs via two steps: the initial formation of a neutral hydrogen molecule, followed by the abstraction of a proton from the remaining CHOH 2+ fragment by the roaming H 2 molecule. This reaction has similarities to the H 2+H 2 + mechanism leading to formation of H 3 + in the universe. These exotic chemical reaction mechanisms, involving roaming H 2 molecules, are found to occur in the ~100 fs timescale. Roaming molecule reactions may help to explain unlikely chemical processes, involving dissociation and formation of multiple chemical bonds, occurring under strong laser fields.
Authors:
 [1] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [3]
  1. Michigan State Univ., East Lansing, MI (United States). Dept. of Chemistry
  2. Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics
  3. Michigan State Univ., East Lansing, MI (United States). Dept. of Chemistry and Dept. of Physics and Astronomy
Publication Date:
Grant/Contract Number:
SC0002325; FG02-86ER13491; FG02-09ER16115; CHE-1565634
Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Michigan State Univ., East Lansing, MI (United States); Kansas State Univ., Manhattan, KS (United States)
Sponsoring Org:
USDOE; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 74 ATOMIC AND MOLECULAR PHYSICS; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Atomic and molecular interactions with photons; Chemical physics; Galaxies and clusters; Reaction kinetics and dynamics
OSTI Identifier:
1430206

Ekanayake, Nagitha, Nairat, Muath, Kaderiya, Balram, Feizollah, Peyman, Jochim, Bethany, Severt, Travis, Berry, Ben, Pandiri, Kanaka Raju, Carnes, Kevin D., Pathak, Shashank, Rolles, Daniel, Rudenko, Artem, Ben-Itzhak, Itzik, Mancuso, Christopher A., Fales, B. Scott, Jackson, James E., Levine, Benjamin G., and Dantus, Marcos. Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields. United States: N. p., Web. doi:10.1038/s41598-017-04666-w.
Ekanayake, Nagitha, Nairat, Muath, Kaderiya, Balram, Feizollah, Peyman, Jochim, Bethany, Severt, Travis, Berry, Ben, Pandiri, Kanaka Raju, Carnes, Kevin D., Pathak, Shashank, Rolles, Daniel, Rudenko, Artem, Ben-Itzhak, Itzik, Mancuso, Christopher A., Fales, B. Scott, Jackson, James E., Levine, Benjamin G., & Dantus, Marcos. Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields. United States. doi:10.1038/s41598-017-04666-w.
Ekanayake, Nagitha, Nairat, Muath, Kaderiya, Balram, Feizollah, Peyman, Jochim, Bethany, Severt, Travis, Berry, Ben, Pandiri, Kanaka Raju, Carnes, Kevin D., Pathak, Shashank, Rolles, Daniel, Rudenko, Artem, Ben-Itzhak, Itzik, Mancuso, Christopher A., Fales, B. Scott, Jackson, James E., Levine, Benjamin G., and Dantus, Marcos. 2017. "Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields". United States. doi:10.1038/s41598-017-04666-w. https://www.osti.gov/servlets/purl/1430206.
@article{osti_1430206,
title = {Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields},
author = {Ekanayake, Nagitha and Nairat, Muath and Kaderiya, Balram and Feizollah, Peyman and Jochim, Bethany and Severt, Travis and Berry, Ben and Pandiri, Kanaka Raju and Carnes, Kevin D. and Pathak, Shashank and Rolles, Daniel and Rudenko, Artem and Ben-Itzhak, Itzik and Mancuso, Christopher A. and Fales, B. Scott and Jackson, James E. and Levine, Benjamin G. and Dantus, Marcos},
abstractNote = {Strong-field laser-matter interactions often lead to exotic chemical reactions. Trihydrogen cation formation from organic molecules is one such case that requires multiple bonds to break and form. Here, we present evidence for the existence of two different reaction pathways for H3+ formation from organic molecules irradiated by a strong-field laser. Assignment of the two pathways was accomplished through analysis of femtosecond time-resolved strong-field ionization and photoion-photoion coincidence measurements carried out on methanol isotopomers, ethylene glycol, and acetone. Ab initio molecular dynamics simulations suggest the formation occurs via two steps: the initial formation of a neutral hydrogen molecule, followed by the abstraction of a proton from the remaining CHOH2+ fragment by the roaming H2 molecule. This reaction has similarities to the H2+H2+ mechanism leading to formation of H3+ in the universe. These exotic chemical reaction mechanisms, involving roaming H2 molecules, are found to occur in the ~100 fs timescale. Roaming molecule reactions may help to explain unlikely chemical processes, involving dissociation and formation of multiple chemical bonds, occurring under strong laser fields.},
doi = {10.1038/s41598-017-04666-w},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {2017},
month = {7}
}

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