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

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Department of Chemistry, Wayne State University, Detroit, Michigan 48202, USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1312052
Grant/Contract Number:
SC0012628
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
The Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 8; Related Information: CHORUS Timestamp: 2018-03-09 12:18:31; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics
Country of Publication:
United States
Language:
English

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.
@article{osti_1312052,
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 = {},
doi = {10.1063/1.4961644},
journal = {The 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1063/1.4961644

Citation Metrics:
Cited by: 1work
Citation information provided by
Web of Science

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  • The hydrogens in protonated acetylene are very mobile and can easily migrate around the C{sub 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{sub 2}CCH{sup +} ion requires only 4 kcal/mol. The effect of circularly polarized light on the migration of hydrogens in oriented C{sub 2}H{sub 3}{sup +} 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 μmmore » cosine squared pulses with peak intensity of 5.6 × 10{sup 13} W/cm{sup 2} and 3.15 × 10{sup 13} W/cm{sup 2}, respectively. These linearly and circularly polarized pulses transfer similar amounts of energy and total angular momentum to C{sub 2}H{sub 3}{sup +}. 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{sub 2} core for circularly polarized light, but only an insignificant amount for linearly polarized light. Over the course of the simulation with circularly polarized light, this corresponds to a propeller-like motion of the three hydrogens around the C{sub 2} core of protonated acetylene.« less
  • Generation of circularly polarized light in the extreme ultraviolet (EUV) spectral region (about 25 eV–250 eV) is highly desirable for applications in spectroscopy and microscopy but very challenging to achieve in a small-scale laboratory. We present a compact apparatus for generation of linearly and circularly polarized EUV radiation from a gas-discharge plasma light source between 50 eV and 70 eV photon energy. In this spectral range, the 3p absorption edges of Fe (54 eV), Co (60 eV), and Ni (67 eV) offer a high magnetic contrast often employed for magneto-optical and electron spectroscopy as well as for magnetic imaging. Wemore » simulated and designed an instrument for generation of linearly and circularly polarized EUV radiation and performed polarimetric measurements of the degree of linear and circular polarization. Furthermore, we demonstrate first measurements of the X-ray magnetic circular dichroism at the Co 3p absorption edge with a plasma-based EUV light source. Our approach opens the door for laboratory-based, element-selective spectroscopy of magnetic materials and spectro-microscopy of ferromagnetic domains.« less
  • A concept of plasma confinement using a combination of inertial and magnetic methods is suggested. A miniature magnetic bottle with the megagauss field can be induced by circularly polarized laser radiation inside a good conductor vessel containing a plasma. The laser pulses also heat the plasma to {similar_to}5 KeV during a few nanoseconds. The Lawson criteria for a DT plasma might be satisfied for densities of the order 5{center_dot}10{sup 21} cm{sup {minus}3} and confinement time about 20 nsec.(AIP) {copyright}{ital American} {ital Institute} {ital of} {ital Physics} 1994
  • We have observed the spin-state interference by measuring the photoelectron spin polarization in the resonant preedge 4d{yields}4f photoemission from magnetized Gd. The photoemission is induced by circularly polarized light which determines one preferential direction of electron spin orientation due to polarization transfer and spin-orbit interaction. Another direction perpendicular to the first one is determined by the target electron spin orientation connected with the target magnetization. We have measured the component of spin polarization perpendicular to those two directions which can only appear due to spin-state interference which implies coherence of the spin states produced by the two mechanisms of themore » photoelectron spin polarization.« less
  • The discovery of meteoritic amino acids with enantiomeric excesses of the L-form (ee {sub L}) has suggested that extraterrestrial organic materials may have contributed to prebiotic chemistry and directed the initial occurrence of the ee {sub L} that further led to homochirality of amino acids on Earth. A proposed mechanism for the origin of ee {sub L} in meteorites involves an asymmetric photochemistry of extraterrestrial ices by UV circularly polarized light (CPL). We have performed the asymmetric synthesis of amino acids on achiral extraterrestrial ice analogs by VUV CPL, investigating the chiral asymmetry transfer at two different evolutionary stages atmore » which the analogs were irradiated (regular ices and/or organic residues) and at two different photon energies (6.6 and 10.2 eV). We identify 16 distinct amino acids and precisely measure the L-enantiomeric excesses using the enantioselective GC × GC-TOFMS technique in five of them: α-alanine, 2,3-diaminopropionic acid, 2-aminobutyric acid, valine, and norvaline, with values ranging from ee {sub L} = –0.20% ± 0.14% to ee {sub L} = –2.54% ± 0.28%. The sign of the induced ee {sub L} depends on the helicity and the energy of CPL, but not on the evolutionary stage of the samples, and is the same for all five considered amino acids. Our results support an astrophysical scenario in which the solar system was formed in a high-mass star-forming region where icy grains were irradiated during the protoplanetary phase by an external source of CPL of a given helicity and a dominant energy, inducing a stereo-specific photochemistry.« less