Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields

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

doi:10.1038/s41598-017-04666-w

Title: Mechanisms and time-resolved dynamics for trihydrogen cation (H₃ +) formation from organic molecules in strong laser fields

Abstract

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.

Authors:

Ekanayake, Nagitha ^[1]; Nairat, Muath ^[1]; Kaderiya, Balram ^[2]; Feizollah, Peyman ^[2]; Jochim, Bethany ^[2]; Severt, Travis ^[2]; Berry, Ben ^[2]; Pandiri, Kanaka Raju ^[2]; Carnes, Kevin D. ^[2]; Pathak, Shashank ^[2]; Rolles, Daniel ^[2]; Rudenko, Artem ^[2]; Ben-Itzhak, Itzik ^[2]; Mancuso, Christopher A. ^[1]; Fales, B. Scott ^[1];

^[1];

^[1]; Dantus, Marcos ^[3]

Michigan State Univ., East Lansing, MI (United States). Dept. of Chemistry
Kansas State Univ., Manhattan, KS (United States). J.R. Macdonald Lab. and Dept. of Physics
Michigan State Univ., East Lansing, MI (United States). Dept. of Chemistry and Dept. of Physics and Astronomy

Publication Date:: Wed Jul 05 00:00:00 EDT 2017

Research Org.:: Michigan State Univ., East Lansing, MI (United States); Kansas State Univ., Manhattan, KS (United States)

Sponsoring Org.:: USDOE; National Science Foundation (NSF)

OSTI Identifier:: 1430206

Grant/Contract Number:: SC0002325; FG02-86ER13491; FG02-09ER16115; CHE-1565634

Resource 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

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

Citation Formats


                    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., 2017. 
Web.  doi:10.1038/s41598-017-04666-w.

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                    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.  https://doi.org/10.1038/s41598-017-04666-w

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                    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. Wed .  
"Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields".  United States.  https://doi.org/10.1038/s41598-017-04666-w.  https://www.osti.gov/servlets/purl/1430206.

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@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         = {Wed Jul 05 00:00:00 EDT 2017},

  month        = {Wed Jul 05 00:00:00 EDT 2017}

}

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Works referenced in this record:

Generating Efficient Quantum Chemistry Codes for Novel Architectures
journal, November 2012

Titov, Alexey V.; Ufimtsev, Ivan S.; Luehr, Nathan
Journal of Chemical Theory and Computation, Vol. 9, Issue 1
DOI: 10.1021/ct300321a

Ultrafast Laser Induced Molecular Alignment and Deformation: Experimental Evidence from Neutral Molecules and from Fragment Ions
journal, October 2003

Comstock, Matthew; Senekerimyan, Vahan; Dantus, Marcos
The Journal of Physical Chemistry A, Vol. 107, Issue 40, p. 8271-8281
DOI: 10.1021/jp0278115

Dissociation and Ionization of $H_{2}^{+}$ by Ultrashort Intense Laser Pulses Probed by Coincidence 3D Momentum Imaging
journal, August 2005

Ben-Itzhak, I.; Wang, P. Q.; Xia, J. F.
Physical Review Letters, Vol. 95, Issue 7
DOI: 10.1103/PhysRevLett.95.073002

On the field ionisation of diatomic molecules by intense laser fields
journal, June 1989

Codling, K.; Frasinski, L. J.; Hatherly, P. A.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 22, Issue 12
DOI: 10.1088/0953-4075/22/12/004

Dissociation of methanol by ion-impact: Breakup dynamics, bond rearrangement and kinetic energy release
journal, September 2008

De, Sankar; Roy, A.; Rajput, Jyoti
International Journal of Mass Spectrometry, Vol. 276, Issue 1
DOI: 10.1016/j.ijms.2008.06.021

High Energy Proton Ejection from Hydrocarbon Molecules Driven by Highly Efficient Field Ionization
journal, April 2011

Roither, Stefan; Xie, Xinhua; Kartashov, Daniil
Physical Review Letters, Vol. 106, Issue 16
DOI: 10.1103/PhysRevLett.106.163001

An atomic orbital-based formulation of the complete active space self-consistent field method on graphical processing units
journal, June 2015

Hohenstein, Edward G.; Luehr, Nathan; Ufimtsev, Ivan S.
The Journal of Chemical Physics, Vol. 142, Issue 22
DOI: 10.1063/1.4921956

Measurements of intense ultrafast laser-driven D $_{3}$ $^{+}$ fragmentation dynamics
journal, September 2012

Sayler, A. M.; McKenna, J.; Gaire, B.
Physical Review A, Vol. 86, Issue 3
DOI: 10.1103/PhysRevA.86.033425

Nanoscale Multireference Quantum Chemistry: Full Configuration Interaction on Graphical Processing Units
journal, September 2015

Fales, B. Scott; Levine, Benjamin G.
Journal of Chemical Theory and Computation, Vol. 11, Issue 10
DOI: 10.1021/acs.jctc.5b00634

Colloquium : Aligning molecules with strong laser pulses
journal, April 2003

Stapelfeldt, Henrik; Seideman, Tamar
Reviews of Modern Physics, Vol. 75, Issue 2
DOI: 10.1103/RevModPhys.75.543

An ab Initio Study of Substituent Effects in [1,3]-Hydrogen Shifts
journal, April 2003

Hudson, Charles E.; McAdoo, David J.
The Journal of Organic Chemistry, Vol. 68, Issue 7
DOI: 10.1021/jo020624i

Metastable decomposition and hydrogen migration of ethane dication produced in an intense femtosecond near-infrared laser field
journal, February 2011

Hoshina, Kennosuke; Kawamura, Haruna; Tsuge, Masashi
The Journal of Chemical Physics, Vol. 134, Issue 6
DOI: 10.1063/1.3549137

Hydrogen migration in methanol studied under asymmetric fs laser irradiation
journal, June 2014

Kotsina, N.; Kaziannis, S.; Kosmidis, C.
Chemical Physics Letters, Vol. 604
DOI: 10.1016/j.cplett.2014.04.040

Molecular Dynamics of Methanol Monocation (CH ₃ OH ⁺ ) in Strong Laser Fields
journal, February 2014

Thapa, Bishnu; Schlegel, H. Bernhard
The Journal of Physical Chemistry A, Vol. 118, Issue 10
DOI: 10.1021/jp410091b

Ejection of triatomic hydrogen molecular ion from methanol in intense laser fields
journal, October 2005

Furukawa, Yusuke; Hoshina, Kennosuke; Yamanouchi, Kaoru
Chemical Physics Letters, Vol. 414, Issue 1-3
DOI: 10.1016/j.cplett.2005.07.108

XIX. Further experiments on positive rays
journal, August 1912

Thomson, J. J.
The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 24, Issue 140
DOI: 10.1080/14786440808637325

Coincidence momentum imaging of ultrafast hydrogen migration in methanol and its isotopomers in intense laser fields
journal, May 2006

Okino, Tomoya; Furukawa, Yusuke; Liu, Peng
Chemical Physics Letters, Vol. 423, Issue 1-3
DOI: 10.1016/j.cplett.2006.03.068

Control of Chemical Reactions by Feedback-Optimized Phase-Shaped Femtosecond Laser Pulses
journal, October 1998

Assion, A.; Baumert, T.; Bergt, M.
Science, Vol. 282, Issue 5390, p. 919-922
DOI: 10.1126/science.282.5390.919

Studies of H+, H+2, and H+3 dissociative ionization fragments from methane, ethane, methanol, ethanol, and some deuterated methanols using electron-impact excitation and a time-of-flight method incorporating mass analysis
journal, January 1979

Burrows, M. D.; Ryan, S. R.; Lamb, W. E.
The Journal of Chemical Physics, Vol. 71, Issue 12
DOI: 10.1063/1.438306

Sequential and nonsequential contributions to double ionization in strong laser fields
journal, February 2000

Weber, Th; Weckenbrock, M.; Staudte, A.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 33, Issue 4
DOI: 10.1088/0953-4075/33/4/104

Interference without an interferometer: a different approach to measuring, compressing, and shaping ultrashort laser pulses
journal, January 2008

Coello, Yves; Lozovoy, Vadim V.; Gunaratne, Tissa C.
Journal of the Optical Society of America B, Vol. 25, Issue 6
DOI: 10.1364/JOSAB.25.00A140

Ejection dynamics of hydrogen molecular ions from methanol in intense laser fields
journal, June 2006

Okino, T.; Furukawa, Y.; Liu, P.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 39, Issue 13
DOI: 10.1088/0953-4075/39/13/S24

Order of Magnitude Dissociative Ionization Enhancement Observed for Pulses with High Order Dispersion
journal, October 2016

Nairat, Muath; Lozovoy, Vadim V.; Dantus, Marcos
The Journal of Physical Chemistry A, Vol. 120, Issue 43
DOI: 10.1021/acs.jpca.6b08659

Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics
journal, June 2000

Dörner, R.; Mergel, V.; Jagutzki, O.
Physics Reports, Vol. 330, Issue 2-3
DOI: 10.1016/S0370-1573(99)00109-X

Quantum Chemistry on Graphical Processing Units. 3. Analytical Energy Gradients, Geometry Optimization, and First Principles Molecular Dynamics
journal, August 2009

Ufimtsev, Ivan S.; Martinez, Todd J.
Journal of Chemical Theory and Computation, Vol. 5, Issue 10
DOI: 10.1021/ct9003004

Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers
journal, October 1995

Zuo, T.; Bandrauk, A. D.
Physical Review A, Vol. 52, Issue 4
DOI: 10.1103/PhysRevA.52.R2511

Polyatomic Molecules under Intense Femtosecond Laser Irradiation
journal, November 2014

Konar, Arkaprabha; Shu, Yinan; Lozovoy, Vadim V.
The Journal of Physical Chemistry A, Vol. 118, Issue 49
DOI: 10.1021/jp505498t

Photodissociation Dynamics of Acetophenone and Its Derivatives with Intense Nonresonant Femtosecond Pulses
journal, March 2011

Zhu, Xin; Lozovoy, Vadim V.; Shah, Jay D.
The Journal of Physical Chemistry A, Vol. 115, Issue 8
DOI: 10.1021/jp1029486

Communication: Long-lived neutral H ₂ in hydrogen migration within methanol dication
journal, November 2013

Nakai, K.; Kato, T.; Kono, H.
The Journal of Chemical Physics, Vol. 139, Issue 18
DOI: 10.1063/1.4830397

Coincidence studies of doubly charged ions formed by 30.4 nm photoionization
journal, February 1985

Curtis, D. M.; Eland, J. H. D.
International Journal of Mass Spectrometry and Ion Processes, Vol. 63, Issue 2-3
DOI: 10.1016/0168-1176(85)80028-8

Quantitative investigation of the multiphoton intrapulse interference phase scan method for simultaneous phase measurement and compensation of femtosecond laser pulses
journal, January 2006

Xu, Bingwei; Gunn, Jess M.; Cruz, Johanna M. Dela
Journal of the Optical Society of America B, Vol. 23, Issue 4, p. 750-759
DOI: 10.1364/JOSAB.23.000750

Efficient ejection of H3+ from hydrocarbon molecules induced by ultrashort intense laser fields
journal, September 2008

Hoshina, Kennosuke; Furukawa, Yusuke; Okino, Tomoya
The Journal of Chemical Physics, Vol. 129, Issue 10
DOI: 10.1063/1.2973588

Coincidence momentum imaging of ejection of hydrogen molecular ions from methanol in intense laser fields
journal, February 2006

Okino, Tomoya; Furukawa, Yusuke; Liu, Peng
Chemical Physics Letters, Vol. 419, Issue 1-3
DOI: 10.1016/j.cplett.2005.11.059

Double photoionization of SO2 and fragmentation spectroscopy of SO2++ studied by a photoion-photoion coincidence method
journal, August 1984

Dujardin, Gérald; Leach, Sydney; Dutuit, Odile
Chemical Physics, Vol. 88, Issue 3
DOI: 10.1016/0301-0104(84)87001-9

Resonant structures in the low-energy electron continuum for single ionization of atoms in the tunnelling regime
journal, December 2004

Rudenko, A.; Zrost, K.; Schröter, C. D.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 37, Issue 24
DOI: 10.1088/0953-4075/37/24/L03

Atomic structure dependence of nonsequential double ionization of He, Ne and Ar in strong laser pulses
journal, April 2004

Jesus, V. L. B. de; Feuerstein, B.; Zrost, K.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 37, Issue 8
DOI: 10.1088/0953-4075/37/8/L03

Phase dependence of OD+, HOD+, and H3+ ions released from the deuterated dication of methanol under ω/2ω laser field irradiation
journal, April 2015

Kotsina, N.; Kaziannis, S.; Kosmidis, C.
International Journal of Mass Spectrometry, Vol. 380
DOI: 10.1016/j.ijms.2015.03.001

Fragmentation dynamics of the methanol dication
journal, September 2008

Kushawaha, R. K.; Bapat, B.
Chemical Physics Letters, Vol. 463, Issue 1-3
DOI: 10.1016/j.cplett.2008.08.019

Optical studies of inertially confined molecular iodine ions
journal, May 1992

Strickland, D. T.; Beaudoin, Y.; Dietrich, P.
Physical Review Letters, Vol. 68, Issue 18
DOI: 10.1103/PhysRevLett.68.2755

Recoil-ion and electron momentum spectroscopy: reaction-microscopes
journal, August 2003

Ullrich, J.; Moshammer, R.; Dorn, A.
Reports on Progress in Physics, Vol. 66, Issue 9
DOI: 10.1088/0034-4885/66/9/203

LASER CHEMISTRY AND PHYSICS: The Next Frontier
journal, March 2002

Yamanouchi, K.
Science, Vol. 295, Issue 5560
DOI: 10.1126/science.1068449

Dynamic and geometric laser-induced alignment of molecules in intense laser fields
journal, July 1998

Posthumus, J. H.; Plumridge, J.; Thomas, M. K.
Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 31, Issue 13
DOI: 10.1088/0953-4075/31/13/002

Electrophilic reactions at single bonds. XI. Hydrogen-deuterium exchange of molecular hydrogen and deuterium in superacids involving isomeric triatomic (hydrogen, deuterium) (+) ions
journal, July 1973

Olah, George A.; Shen, Jacob.; Schlosberg, Richard H.
Journal of the American Chemical Society, Vol. 95, Issue 15
DOI: 10.1021/ja00796a030

Control of Molecular Fragmentation Using Shaped Femtosecond Pulses
journal, May 2008

Lozovoy, Vadim V.; Zhu, Xin; Gunaratne, Tissa C.
The Journal of Physical Chemistry A, Vol. 112, Issue 17
DOI: 10.1021/jp071691p

Kinetic energy release distributions in mass spectrometry
journal, January 2001

Laskin, J.; Lifshitz, C.
Journal of Mass Spectrometry, Vol. 36, Issue 5
DOI: 10.1002/jms.164

Pathways and reduced-dimension five-dimensional potential energy surface for the reactions H3++CO→H2+HCO+ and H3++CO→H2+HOC+
journal, December 2008

Li, Hui; Hirano, Tsuneo; Amano, Takayoshi
The Journal of Chemical Physics, Vol. 129, Issue 24
DOI: 10.1063/1.3041494

Coulomb explosion of $N_{2}$ and ${CO}_{2}$ using linearly and circularly polarized femtosecond laser pulses
journal, April 1999

Hering, Ph.; Cornaggia, C.
Physical Review A, Vol. 59, Issue 4
DOI: 10.1103/PhysRevA.59.2836

High Energy Proton Ejection from Hydrocarbon Molecules Driven by Highly Efficient Field Ionization
book, January 2012

Roither, S.; Xie, X.; Kartashov, D.
Springer Proceedings in Physics
DOI: 10.1007/978-3-642-28948-4_56

High energy proton ejection from hydrocarbon molecules driven by highly efficient field ionization
journal, November 2012

Roither, S.; Xie, X.; Kartashov, D.
Journal of Physics: Conference Series, Vol. 388, Issue 3
DOI: 10.1088/1742-6596/388/3/032063

An ab initio Study of Substituent Effects in [1,3]-Hydrogen Shifts.
journal, July 2003

Hudson, Charles E.; McAdoo, David J.
ChemInform, Vol. 34, Issue 29
DOI: 10.1002/chin.200329025

The Next Frontier
book, January 2008

Bosilca, George
Recent Advances in Parallel Virtual Machine and Message Passing Interface
DOI: 10.1007/978-3-540-87475-1_1

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journal, March 2018

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DOI: 10.1038/s42004-017-0006-7

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journal, January 2018

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DOI: 10.1039/c8cp05780j

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RSC Advances, Vol. 9, Issue 29
DOI: 10.1039/c9ra02003a

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DOI: 10.1063/1.5065387

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journal, January 2019

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The Journal of Chemical Physics, Vol. 150, Issue 4
DOI: 10.1063/1.5070067

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journal, May 2019

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The Journal of Chemical Physics, Vol. 150, Issue 20
DOI: 10.1063/1.5088690

Strong-field control of H3+ production from methanol dications: Selecting between local and extended formation mechanisms
journal, February 2020

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The Journal of Chemical Physics, Vol. 152, Issue 5
DOI: 10.1063/1.5129946

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journal, May 2019

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Physical Review A, Vol. 99, Issue 5
DOI: 10.1103/physreva.99.053412

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Title: Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields

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Generating Efficient Quantum Chemistry Codes for Novel Architectures journal, November 2012

Ultrafast Laser Induced Molecular Alignment and Deformation: Experimental Evidence from Neutral Molecules and from Fragment Ions journal, October 2003

Dissociation and Ionization of H 2 + by Ultrashort Intense Laser Pulses Probed by Coincidence 3D Momentum Imaging journal, August 2005

On the field ionisation of diatomic molecules by intense laser fields journal, June 1989

Dissociation of methanol by ion-impact: Breakup dynamics, bond rearrangement and kinetic energy release journal, September 2008

High Energy Proton Ejection from Hydrocarbon Molecules Driven by Highly Efficient Field Ionization journal, April 2011

An atomic orbital-based formulation of the complete active space self-consistent field method on graphical processing units journal, June 2015

Measurements of intense ultrafast laser-driven D 3 + fragmentation dynamics journal, September 2012

Nanoscale Multireference Quantum Chemistry: Full Configuration Interaction on Graphical Processing Units journal, September 2015

Colloquium : Aligning molecules with strong laser pulses journal, April 2003

An ab Initio Study of Substituent Effects in [1,3]-Hydrogen Shifts journal, April 2003

Metastable decomposition and hydrogen migration of ethane dication produced in an intense femtosecond near-infrared laser field journal, February 2011

Hydrogen migration in methanol studied under asymmetric fs laser irradiation journal, June 2014

Molecular Dynamics of Methanol Monocation (CH 3 OH + ) in Strong Laser Fields journal, February 2014

Ejection of triatomic hydrogen molecular ion from methanol in intense laser fields journal, October 2005

XIX. Further experiments on positive rays journal, August 1912

Coincidence momentum imaging of ultrafast hydrogen migration in methanol and its isotopomers in intense laser fields journal, May 2006

Control of Chemical Reactions by Feedback-Optimized Phase-Shaped Femtosecond Laser Pulses journal, October 1998

Studies of H+, H+2, and H+3 dissociative ionization fragments from methane, ethane, methanol, ethanol, and some deuterated methanols using electron-impact excitation and a time-of-flight method incorporating mass analysis journal, January 1979

Sequential and nonsequential contributions to double ionization in strong laser fields journal, February 2000

Interference without an interferometer: a different approach to measuring, compressing, and shaping ultrashort laser pulses journal, January 2008

Ejection dynamics of hydrogen molecular ions from methanol in intense laser fields journal, June 2006

Order of Magnitude Dissociative Ionization Enhancement Observed for Pulses with High Order Dispersion journal, October 2016

Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics journal, June 2000

Quantum Chemistry on Graphical Processing Units. 3. Analytical Energy Gradients, Geometry Optimization, and First Principles Molecular Dynamics journal, August 2009

Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers journal, October 1995

Polyatomic Molecules under Intense Femtosecond Laser Irradiation journal, November 2014

Photodissociation Dynamics of Acetophenone and Its Derivatives with Intense Nonresonant Femtosecond Pulses journal, March 2011

Communication: Long-lived neutral H 2 in hydrogen migration within methanol dication journal, November 2013

Coincidence studies of doubly charged ions formed by 30.4 nm photoionization journal, February 1985

Quantitative investigation of the multiphoton intrapulse interference phase scan method for simultaneous phase measurement and compensation of femtosecond laser pulses journal, January 2006

Efficient ejection of H3+ from hydrocarbon molecules induced by ultrashort intense laser fields journal, September 2008

Coincidence momentum imaging of ejection of hydrogen molecular ions from methanol in intense laser fields journal, February 2006

Double photoionization of SO2 and fragmentation spectroscopy of SO2++ studied by a photoion-photoion coincidence method journal, August 1984

Resonant structures in the low-energy electron continuum for single ionization of atoms in the tunnelling regime journal, December 2004

Atomic structure dependence of nonsequential double ionization of He, Ne and Ar in strong laser pulses journal, April 2004

Phase dependence of OD+, HOD+, and H3+ ions released from the deuterated dication of methanol under ω/2ω laser field irradiation journal, April 2015

Fragmentation dynamics of the methanol dication journal, September 2008

Optical studies of inertially confined molecular iodine ions journal, May 1992

Recoil-ion and electron momentum spectroscopy: reaction-microscopes journal, August 2003

LASER CHEMISTRY AND PHYSICS: The Next Frontier journal, March 2002

Dynamic and geometric laser-induced alignment of molecules in intense laser fields journal, July 1998

Electrophilic reactions at single bonds. XI. Hydrogen-deuterium exchange of molecular hydrogen and deuterium in superacids involving isomeric triatomic (hydrogen, deuterium) (+) ions journal, July 1973

Control of Molecular Fragmentation Using Shaped Femtosecond Pulses journal, May 2008

Kinetic energy release distributions in mass spectrometry journal, January 2001

Pathways and reduced-dimension five-dimensional potential energy surface for the reactions H3++CO→H2+HCO+ and H3++CO→H2+HOC+ journal, December 2008

Coulomb explosion of N 2 and CO 2 using linearly and circularly polarized femtosecond laser pulses journal, April 1999

High Energy Proton Ejection from Hydrocarbon Molecules Driven by Highly Efficient Field Ionization book, January 2012

High energy proton ejection from hydrocarbon molecules driven by highly efficient field ionization journal, November 2012

An ab initio Study of Substituent Effects in [1,3]-Hydrogen Shifts. journal, July 2003

The Next Frontier book, January 2008

H2 roaming chemistry and the formation of H3+ from organic molecules in strong laser fields journal, December 2018

Time-resolved molecular dynamics of single and double hydrogen migration in ethanol journal, June 2019

Coherent vibrations in methanol cation probed by periodic H3+ ejection after double ionization journal, March 2018

Dissociation of [HCCH] 2+ to H 2 + and C 2 + : a benchmark reaction involving H migration, H–H combination, and C–H bond cleavage journal, January 2018

Theoretical and experimental studies on hydrogen migration in dissociative ionization of the methanol monocation to molecular ions H 3 + and H 2 O + journal, January 2019

Substituent effects on H 3 + formation via H 2 roaming mechanisms from organic molecules under strong-field photodissociation journal, December 2018

Quantum coherent control of H 3 + formation in strong fields journal, January 2019

Proton migration in hydrocarbons induced by slow highly charged ion impact journal, May 2019

Strong-field control of H3+ production from methanol dications: Selecting between local and extended formation mechanisms journal, February 2020

Strong-field-induced bond rearrangement in triatomic molecules journal, May 2019

H2 roaming chemistry and the formation of H3+ from organic molecules in strong laser fields journal, December 2018

Time-resolved molecular dynamics of single and double hydrogen migration in ethanol journal, June 2019

Title: Mechanisms and time-resolved dynamics for trihydrogen cation (H₃ +) formation from organic molecules in strong laser fields

Generating Efficient Quantum Chemistry Codes for Novel Architectures
journal, November 2012

Ultrafast Laser Induced Molecular Alignment and Deformation: Experimental Evidence from Neutral Molecules and from Fragment Ions
journal, October 2003

Dissociation and Ionization of $H_{2}^{+}$ by Ultrashort Intense Laser Pulses Probed by Coincidence 3D Momentum Imaging
journal, August 2005

On the field ionisation of diatomic molecules by intense laser fields
journal, June 1989

Dissociation of methanol by ion-impact: Breakup dynamics, bond rearrangement and kinetic energy release
journal, September 2008

High Energy Proton Ejection from Hydrocarbon Molecules Driven by Highly Efficient Field Ionization
journal, April 2011

An atomic orbital-based formulation of the complete active space self-consistent field method on graphical processing units
journal, June 2015

Measurements of intense ultrafast laser-driven D $_{3}$ $^{+}$ fragmentation dynamics
journal, September 2012

Nanoscale Multireference Quantum Chemistry: Full Configuration Interaction on Graphical Processing Units
journal, September 2015

Colloquium : Aligning molecules with strong laser pulses
journal, April 2003

An ab Initio Study of Substituent Effects in [1,3]-Hydrogen Shifts
journal, April 2003

Metastable decomposition and hydrogen migration of ethane dication produced in an intense femtosecond near-infrared laser field
journal, February 2011

Hydrogen migration in methanol studied under asymmetric fs laser irradiation
journal, June 2014

Molecular Dynamics of Methanol Monocation (CH ₃ OH ⁺ ) in Strong Laser Fields
journal, February 2014

Ejection of triatomic hydrogen molecular ion from methanol in intense laser fields
journal, October 2005

XIX. Further experiments on positive rays
journal, August 1912

Coincidence momentum imaging of ultrafast hydrogen migration in methanol and its isotopomers in intense laser fields
journal, May 2006

Control of Chemical Reactions by Feedback-Optimized Phase-Shaped Femtosecond Laser Pulses
journal, October 1998

Studies of H+, H+2, and H+3 dissociative ionization fragments from methane, ethane, methanol, ethanol, and some deuterated methanols using electron-impact excitation and a time-of-flight method incorporating mass analysis
journal, January 1979

Sequential and nonsequential contributions to double ionization in strong laser fields
journal, February 2000

Interference without an interferometer: a different approach to measuring, compressing, and shaping ultrashort laser pulses
journal, January 2008

Ejection dynamics of hydrogen molecular ions from methanol in intense laser fields
journal, June 2006

Order of Magnitude Dissociative Ionization Enhancement Observed for Pulses with High Order Dispersion
journal, October 2016

Cold Target Recoil Ion Momentum Spectroscopy: a ‘momentum microscope’ to view atomic collision dynamics
journal, June 2000

Quantum Chemistry on Graphical Processing Units. 3. Analytical Energy Gradients, Geometry Optimization, and First Principles Molecular Dynamics
journal, August 2009

Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers
journal, October 1995

Polyatomic Molecules under Intense Femtosecond Laser Irradiation
journal, November 2014

Photodissociation Dynamics of Acetophenone and Its Derivatives with Intense Nonresonant Femtosecond Pulses
journal, March 2011

Communication: Long-lived neutral H ₂ in hydrogen migration within methanol dication
journal, November 2013

Coincidence studies of doubly charged ions formed by 30.4 nm photoionization
journal, February 1985

Quantitative investigation of the multiphoton intrapulse interference phase scan method for simultaneous phase measurement and compensation of femtosecond laser pulses
journal, January 2006

Efficient ejection of H3+ from hydrocarbon molecules induced by ultrashort intense laser fields
journal, September 2008

Coincidence momentum imaging of ejection of hydrogen molecular ions from methanol in intense laser fields
journal, February 2006

Double photoionization of SO2 and fragmentation spectroscopy of SO2++ studied by a photoion-photoion coincidence method
journal, August 1984

Resonant structures in the low-energy electron continuum for single ionization of atoms in the tunnelling regime
journal, December 2004

Atomic structure dependence of nonsequential double ionization of He, Ne and Ar in strong laser pulses
journal, April 2004

Phase dependence of OD+, HOD+, and H3+ ions released from the deuterated dication of methanol under ω/2ω laser field irradiation
journal, April 2015

Fragmentation dynamics of the methanol dication
journal, September 2008

Optical studies of inertially confined molecular iodine ions
journal, May 1992

Recoil-ion and electron momentum spectroscopy: reaction-microscopes
journal, August 2003

LASER CHEMISTRY AND PHYSICS: The Next Frontier
journal, March 2002

Dynamic and geometric laser-induced alignment of molecules in intense laser fields
journal, July 1998

Electrophilic reactions at single bonds. XI. Hydrogen-deuterium exchange of molecular hydrogen and deuterium in superacids involving isomeric triatomic (hydrogen, deuterium) (+) ions
journal, July 1973

Control of Molecular Fragmentation Using Shaped Femtosecond Pulses
journal, May 2008

Kinetic energy release distributions in mass spectrometry
journal, January 2001

Pathways and reduced-dimension five-dimensional potential energy surface for the reactions H3++CO→H2+HCO+ and H3++CO→H2+HOC+
journal, December 2008

Coulomb explosion of $N_{2}$ and ${CO}_{2}$ using linearly and circularly polarized femtosecond laser pulses
journal, April 1999

High Energy Proton Ejection from Hydrocarbon Molecules Driven by Highly Efficient Field Ionization
book, January 2012

High energy proton ejection from hydrocarbon molecules driven by highly efficient field ionization
journal, November 2012

An ab initio Study of Substituent Effects in [1,3]-Hydrogen Shifts.
journal, July 2003

The Next Frontier
book, January 2008

H2 roaming chemistry and the formation of H3+ from organic molecules in strong laser fields
journal, December 2018

Time-resolved molecular dynamics of single and double hydrogen migration in ethanol
journal, June 2019

Coherent vibrations in methanol cation probed by periodic H3+ ejection after double ionization
journal, March 2018

Dissociation of [HCCH] ²⁺ to H ₂ ⁺ and C ₂ ⁺ : a benchmark reaction involving H migration, H–H combination, and C–H bond cleavage
journal, January 2018

Theoretical and experimental studies on hydrogen migration in dissociative ionization of the methanol monocation to molecular ions H ₃ ⁺ and H ₂ O ⁺
journal, January 2019

Substituent effects on H ₃ ⁺ formation via H ₂ roaming mechanisms from organic molecules under strong-field photodissociation
journal, December 2018

Quantum coherent control of H ₃ ⁺ formation in strong fields
journal, January 2019

Proton migration in hydrocarbons induced by slow highly charged ion impact
journal, May 2019

Strong-field control of H3+ production from methanol dications: Selecting between local and extended formation mechanisms
journal, February 2020

Strong-field-induced bond rearrangement in triatomic molecules
journal, May 2019

H2 roaming chemistry and the formation of H3+ from organic molecules in strong laser fields
journal, December 2018

Time-resolved molecular dynamics of single and double hydrogen migration in ethanol
journal, June 2019