Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light
Abstract
The hydrogens in protonated acetylene are very mobile and can easily migrate around the C2 core by moving between classical and non-classical structures of the cation. The lowest energy structure is the T-shaped, non-classical cation with a hydrogen bridging the two carbons. Conversion to the classical H2CCH+ ion requires only 4 kcal/mol. The effect of circularly polarized light on the migration of hydrogens in oriented C2H3+ has been simulated by Born-Oppenheimer molecular dynamics. Classical trajectory calculations were carried out with the M062X/6-311+G(3df,2pd) level of theory using linearly and circularly polarized 32 cycle 7 μm cosine squared pulses with peak intensity of 5.6 × 1013 W/cm2 and 3.15 × 1013 W/cm2, respectively. These linearly and circularly polarized pulses transfer similar amounts of energy and total angular momentum to C2H3+. The average angular momentum vectors of the three hydrogens show opposite directions of rotation for right and left circularly polarized light, but no directional preference for linearly polarized light. This difference results in an appreciable amount of angular displacement of the three hydrogens relative to the C2 core for circularly polarized light, but only an insignificant amount for linearly polarized light. In conclusion, over the course of the simulation with circularly polarizedmore »
- Authors:
-
- Wayne State Univ., Detroit, MI (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Wayne State Univ., Detroit, MI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1467879
- Alternate Identifier(s):
- OSTI ID: 1312052
- Grant/Contract Number:
- SC0012628
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 145; Journal Issue: 8; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 08 HYDROGEN
Citation Formats
Shi, Xuetao, Li, Wen, and Schlegel, H. Bernhard. Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light. United States: N. p., 2016.
Web. doi:10.1063/1.4961644.
Shi, Xuetao, Li, Wen, & Schlegel, H. Bernhard. Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light. United States. https://doi.org/10.1063/1.4961644
Shi, Xuetao, Li, Wen, and Schlegel, H. Bernhard. Tue .
"Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light". United States. https://doi.org/10.1063/1.4961644. https://www.osti.gov/servlets/purl/1467879.
@article{osti_1467879,
title = {Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light},
author = {Shi, Xuetao and Li, Wen and Schlegel, H. Bernhard},
abstractNote = {The hydrogens in protonated acetylene are very mobile and can easily migrate around the C2 core by moving between classical and non-classical structures of the cation. The lowest energy structure is the T-shaped, non-classical cation with a hydrogen bridging the two carbons. Conversion to the classical H2CCH+ ion requires only 4 kcal/mol. The effect of circularly polarized light on the migration of hydrogens in oriented C2H3+ has been simulated by Born-Oppenheimer molecular dynamics. Classical trajectory calculations were carried out with the M062X/6-311+G(3df,2pd) level of theory using linearly and circularly polarized 32 cycle 7 μm cosine squared pulses with peak intensity of 5.6 × 1013 W/cm2 and 3.15 × 1013 W/cm2, respectively. These linearly and circularly polarized pulses transfer similar amounts of energy and total angular momentum to C2H3+. The average angular momentum vectors of the three hydrogens show opposite directions of rotation for right and left circularly polarized light, but no directional preference for linearly polarized light. This difference results in an appreciable amount of angular displacement of the three hydrogens relative to the C2 core for circularly polarized light, but only an insignificant amount for linearly polarized light. In conclusion, over the course of the simulation with circularly polarized light, this corresponds to a propeller-like motion of the three hydrogens around the C2 core of protonated acetylene.},
doi = {10.1063/1.4961644},
journal = {Journal of Chemical Physics},
number = 8,
volume = 145,
place = {United States},
year = {Tue Aug 30 00:00:00 EDT 2016},
month = {Tue Aug 30 00:00:00 EDT 2016}
}
Web of Science
Works referenced in this record:
Quartic Force Field Rovibrational Analysis of Protonated Acetylene, C 2 H 3 + , and Its Isotopologues
journal, August 2014
- Fortenberry, Ryan C.; Huang, Xinchuan; Crawford, T. Daniel
- The Journal of Physical Chemistry A, Vol. 118, Issue 34
Molecular Dynamics in Strong Laser Fields: A New Algorithm for ab Initio Classical Trajectories
journal, July 2013
- Schlegel, H. Bernhard
- Journal of Chemical Theory and Computation, Vol. 9, Issue 8
The energy separation between the classical and nonclassical isomers of protonated acetylene. An extensive study in one‐ and n ‐particle space
journal, June 1991
- Lindh, Roland; Rice, Julia E.; Lee, Timothy J.
- The Journal of Chemical Physics, Vol. 94, Issue 12
Experimental evidence for anomalous nuclear delocalization in
journal, December 1993
- Vager, Z.; Zajfman, D.; Graber, T.
- Physical Review Letters, Vol. 71, Issue 26
On non‐RRKM unimolecular kinetics: Molecules in general, and CH 3 NC in particular
journal, November 1973
- Bunker, Don L.; Hase, W. L.
- The Journal of Chemical Physics, Vol. 59, Issue 9
The Effect of Quantum and Thermal Fluctuations on the Structure of the Floppy Molecule C2H3+
journal, January 1996
- Marx, D.; Parrinello, M.
- Science, Vol. 271, Issue 5246
Ab initio classical trajectories on the Born–Oppenheimer surface: Updating methods for Hessian-based integrators
journal, November 1999
- Bakken, Vebjørn; Millam, John M.; Bernhard Schlegel, H.
- The Journal of Chemical Physics, Vol. 111, Issue 19
Protonated acetylene revisited
journal, January 2007
- Psciuk, Brian T.; Benderskii, Victor A.; Schlegel, H. Bernhard
- Theoretical Chemistry Accounts, Vol. 118, Issue 1
The Roaming Atom: Straying from the Reaction Path in Formaldehyde Decomposition
journal, November 2004
- Townsend, D.
- Science, Vol. 306, Issue 5699
Infrared Spectroscopy of Carboions. 8. Hollow Cathode Spectroscopy of Protonated Acetylene, C2H3+
journal, October 1995
- Gabrys, C. M.; Uy, D.; Jagod, M. -F.
- The Journal of Physical Chemistry, Vol. 99, Issue 42
Ultrafast hydrogen scrambling in methylacetylene and methyl-d3-acetylene ions induced by intense laser fields
journal, January 2012
- Okino, Tomoya; Watanabe, Anri; Xu, Huailiang
- Physical Chemistry Chemical Physics, Vol. 14, Issue 30
Effect of Laser Parameters on Ultrafast Hydrogen Migration in Methanol Studied by Coincidence Momentum Imaging
journal, October 2011
- Xu, Huailiang; Okino, Tomoya; Kudou, Tatsuya
- The Journal of Physical Chemistry A, Vol. 116, Issue 11
Bond-Selective Dissociation of Polyatomic Cations in Mid-Infrared Strong Fields
journal, October 2013
- Lee, Suk Kyoung; Schlegel, H. Bernhard; Li, Wen
- The Journal of Physical Chemistry A, Vol. 117, Issue 44
Ultrafast Extreme Ultraviolet Induced Isomerization of Acetylene Cations
journal, December 2010
- Jiang, Y. H.; Rudenko, A.; Herrwerth, O.
- Physical Review Letters, Vol. 105, Issue 26
Ultrafast hydrogen migration in allene in intense laser fields: Evidence of two-body Coulomb explosion
journal, February 2009
- Xu, Huailiang; Okino, Tomoya; Yamanouchi, Kaoru
- Chemical Physics Letters, Vol. 469, Issue 4-6
HCO+ dissociation in a strong laser field: An ab initio classical trajectory study
journal, May 2012
- Lee, Suk Kyoung; Li, Wen; Bernhard Schlegel, H.
- Chemical Physics Letters, Vol. 536
Structural Dynamics of Protonated Methane and Acetylene
journal, February 1995
- Tse, John S.; Klug, Dennis D.; Laasonen, Kari
- Physical Review Letters, Vol. 74, Issue 6
Molecular dynamics of methanol cation (CH 3 OH + ) in strong fields: Comparison of 800 nm and 7 μm laser fields
journal, August 2014
- Thapa, Bishnu; Schlegel, H. Bernhard
- Chemical Physics Letters, Vol. 610-611
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
Vibrational Energy Flow in Highly Excited Molecules: Role of Intramolecular Vibrational Redistribution
journal, January 1996
- Nesbitt, David J.; Field, Robert W.
- The Journal of Physical Chemistry, Vol. 100, Issue 31
Two-body Coulomb explosion and hydrogen migration in methanol induced by intense 7 and 21fs laser pulses
journal, September 2007
- Itakura, Ryuji; Liu, Peng; Furukawa, Yusuke
- The Journal of Chemical Physics, Vol. 127, Issue 10
Self‐consistent molecular orbital methods. XX. A basis set for correlated wave functions
journal, January 1980
- Krishnan, R.; Binkley, J. S.; Seeger, R.
- The Journal of Chemical Physics, Vol. 72, Issue 1
Classical Dynamics Methods for High Energy Vibrational Spectroscopy
journal, October 1992
- Gomez Llorente, J. M.; Pollak, E.
- Annual Review of Physical Chemistry, Vol. 43, Issue 1
Steering Proton Migration in Hydrocarbons Using Intense Few-Cycle Laser Fields
journal, May 2016
- Kübel, M.; Siemering, R.; Burger, C.
- Physical Review Letters, Vol. 116, Issue 19
Theoretical study of structures and energies of acetylene, ethylene, and vinyl radical and cation
journal, June 1988
- Curtiss, Larry A.; Pople, John A.
- The Journal of Chemical Physics, Vol. 88, Issue 12
Infrared spectroscopy of carbo‐ions. V. Classical vs nonclassical structure of protonated acetylene C 2 H + 3
journal, November 1989
- Crofton, Mark W.; Jagod, Mary‐Frances; Rehfuss, Brent D.
- The Journal of Chemical Physics, Vol. 91, Issue 9
The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals
journal, July 2007
- Zhao, Yan; Truhlar, Donald G.
- Theoretical Chemistry Accounts, Vol. 120, Issue 1-3
Roaming Radicals
journal, May 2011
- Bowman, Joel M.; Shepler, Benjamin C.
- Annual Review of Physical Chemistry, Vol. 62, Issue 1
A CAS SCF CI study of the hydrogen migration potential in protonated acetylene, C2H3+
journal, January 1987
- Lindh, Roland; Roos, Bjorn O.; Kraemer, Wolfgang P.
- Chemical Physics Letters, Vol. 139, Issue 5
Self‐consistent molecular orbital methods 25. Supplementary functions for Gaussian basis sets
journal, April 1984
- Frisch, Michael J.; Pople, John A.; Binkley, J. Stephen
- The Journal of Chemical Physics, Vol. 80, Issue 7
Potential energy surface and MULTIMODE vibrational analysis of C2H3+
journal, December 2006
- Sharma, Amit R.; Wu, Jiayan; Braams, Bastiaan J.
- The Journal of Chemical Physics, Vol. 125, Issue 22
Experimental versus simulated Coulomb-explosion images of flexible molecules: Structure of protonated acetylene
journal, February 2003
- Knoll, Lars; Vager, Zeev; Marx, Dominik
- Physical Review A, Vol. 67, Issue 2
Multiphoton Dissociation of Polyatomic Molecules
journal, October 1979
- Schulz, P. A.; Sudb¢, A. S.; Krajnovich, D. J.
- Annual Review of Physical Chemistry, Vol. 30, Issue 1
Photoelectron-Photoion Momentum Spectroscopy as a Clock for Chemical Rearrangements: Isomerization of the Di-Cation of Acetylene to the Vinylidene Configuration
journal, June 2003
- Osipov, T.; Cocke, C. L.; Prior, M. H.
- Physical Review Letters, Vol. 90, Issue 23
Controlling Chemical Reactions by Short, Intense Mid-Infrared Laser Pulses: Comparison of Linear and Circularly Polarized Light in Simulations of ClCHO + Fragmentation
journal, February 2016
- Shi, Xuetao; Thapa, Bishnu; Li, Wen
- The Journal of Physical Chemistry A, Vol. 120, Issue 7
The classical and nonclassical forms of protonated acetylene, C 2 H + 3 . Structures, vibrational frequencies, and infrared intensities from explicitly correlated wave functions
journal, September 1986
- Lee, Timothy J.; Schaefer, Henry F.
- The Journal of Chemical Physics, Vol. 85, Issue 6
Molecular Dynamics of Methylamine, Methanol, and Methyl Fluoride Cations in Intense 7 Micron Laser Fields
journal, October 2014
- Thapa, Bishnu; Schlegel, H. Bernhard
- The Journal of Physical Chemistry A, Vol. 118, Issue 43
Communication: Two stages of ultrafast hydrogen migration in methanol driven by intense laser fields
journal, August 2010
- Xu, Huailiang; Marceau, Claude; Nakai, Katsunori
- The Journal of Chemical Physics, Vol. 133, Issue 7
Roaming Atoms and Radicals: A New Mechanism in Molecular Dissociation
journal, July 2008
- Suits, Arthur G.
- Accounts of Chemical Research, Vol. 41, Issue 7
A Reaction Accelerator: Mid-infrared Strong Field Dissociation Yields Mode-Selective Chemistry
journal, August 2012
- Lee, Suk Kyoung; Suits, Arthur G.; Schlegel, H. Bernhard
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 18
Tabletop imaging of structural evolutions in chemical reactions demonstrated for the acetylene cation
journal, July 2014
- Ibrahim, Heide; Wales, Benji; Beaulieu, Samuel
- Nature Communications, Vol. 5, Issue 1
The roaming atom pathway in formaldehyde decomposition
journal, July 2006
- Lahankar, Sridhar A.; Chambreau, Steven D.; Townsend, Dave
- The Journal of Chemical Physics, Vol. 125, Issue 4
Higher-accuracy schemes for approximating the Hessian from electronic structure calculations in chemical dynamics simulations
journal, August 2010
- Wu, H.; Rahman, M.; Wang, J.
- The Journal of Chemical Physics, Vol. 133, Issue 7
Works referencing / citing this record:
Controlling the strong field fragmentation of ClCHO + using two laser pulses -an ab initio molecular dynamics simulation: Controlling the strong field fragmentation of ClCHO + using two laser pulses -an ab initio molecular dynamics simulation
journal, October 2018
- Shi, Xuetao; Schlegel, H. Bernhard
- Journal of Computational Chemistry, Vol. 40, Issue 1