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Title: 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 C 2 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 H 2CCH + ion requires only 4 kcal/mol. The effect of circularly polarized light on the migration of hydrogens in oriented C 2H 3 + 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 × 10 13 W/cm 2 and 3.15 × 10 13 W/cm 2, respectively. These linearly and circularly polarized pulses transfer similar amounts of energy and total angular momentum to C 2H3 +. 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 C 2 core for circularly polarized light, but only an insignificant amount for linearlymore » 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 C 2 core of protonated acetylene.« less

Authors:
 [1];  [1]; ORCiD logo [1]
  1. 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) (SC-22)
OSTI Identifier:
1467879
Alternate Identifier(s):
OSTI ID: 1312052
Grant/Contract Number:  
SC0012628
Resource Type:
Journal Article: 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. doi: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. doi: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}
}

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