Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light

Shi, Xuetao; Li, Wen; Schlegel, H. Bernhard

doi:10.1063/1.4961644

Title: Computational simulations of hydrogen circular migration in protonated acetylene induced by circularly polarized light

Journal Article · Tue Aug 30 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4961644· OSTI ID:1467879

Shi, Xuetao ^[1]; Li, Wen ^[1];

^[1]

Wayne State Univ., Detroit, MI (United States). Dept. of Chemistry

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.

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Research Organization:: Wayne State Univ., Detroit, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012628

OSTI ID:: 1467879

Alternate ID(s):: OSTI ID: 1312052

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 8; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 4 works

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