Collision dynamics of symmetric top molecules: A comparison of the rotationally inelastic scattering of CD{sub 3} and ND{sub 3} with He
Abstract
We compare rotationally inelastic scattering of deuterated methyl radicals (CD{sub 3}) and ammonia (ND{sub 3}) in collisions with helium using close-coupling quantum-mechanical scattering calculations performed with ab initio potential energy surfaces (PESs). The theoretical methods have been rigorously tested against angle-resolved experimental measurements obtained using crossed molecular beam apparatuses in combination with velocity map imaging [O. Tkáč, A. G. Sage, S. J. Greaves, A. J. Orr-Ewing, P. J. Dagdigian, Q. Ma, and M. H. Alexander, Chem. Sci. 4, 4199 (2013); O. Tkáč, A. K. Saha, J. Onvlee, C.-H. Yang, G. Sarma, C. K. Bishwakarma, S. Y. T. van de Meerakker, A. van der Avoird, D. H. Parker, and A. J. Orr-Ewing, Phys. Chem. Chem. Phys. 16, 477 (2014)]. Common features of the scattering dynamics of these two symmetric top molecules, one closed-shell and the other an open-shell radical, are identified and discussed. Two types of anisotropies in the PES influence the interaction of an atom with a nonlinear polyatomic molecule. The effects of these anisotropies can be clearly seen in the state-to-state integral cross sections out of the lowest CD{sub 3} rotational levels of each nuclear spin symmetry at a collision energy of 440 cm{sup −1}. Similarities and differences inmore »
- Authors:
-
- School of Chemistry, University of Bristol, Cantock's Close, Bristol BS8 1TS (United Kingdom)
- Department of Chemistry and Biochemistry and Institute for Physical Science and Technology, University of Maryland, College Park, Maryland 20742-2021 (United States)
- Publication Date:
- OSTI Identifier:
- 22253305
- Resource Type:
- Journal Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 13; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; AMMONIA; ANISOTROPY; COLLISIONS; COUPLING; DEUTERIDES; DIFFERENTIAL CROSS SECTIONS; INELASTIC SCATTERING; INTEGRAL CROSS SECTIONS; INTERACTIONS; METHYL RADICALS; MOLECULAR BEAMS; POTENTIAL ENERGY; QUANTUM MECHANICS
Citation Formats
Tkáč, Ondřej, Orr-Ewing, Andrew J., Dagdigian, Paul J., E-mail: pjdagdigian@jhu.edu, Alexander, Millard H., Onvlee, Jolijn, and Avoird, Ad van der, E-mail: avda@theochem.ru.nl. Collision dynamics of symmetric top molecules: A comparison of the rotationally inelastic scattering of CD{sub 3} and ND{sub 3} with He. United States: N. p., 2014.
Web. doi:10.1063/1.4869596.
Tkáč, Ondřej, Orr-Ewing, Andrew J., Dagdigian, Paul J., E-mail: pjdagdigian@jhu.edu, Alexander, Millard H., Onvlee, Jolijn, & Avoird, Ad van der, E-mail: avda@theochem.ru.nl. Collision dynamics of symmetric top molecules: A comparison of the rotationally inelastic scattering of CD{sub 3} and ND{sub 3} with He. United States. https://doi.org/10.1063/1.4869596
Tkáč, Ondřej, Orr-Ewing, Andrew J., Dagdigian, Paul J., E-mail: pjdagdigian@jhu.edu, Alexander, Millard H., Onvlee, Jolijn, and Avoird, Ad van der, E-mail: avda@theochem.ru.nl. 2014.
"Collision dynamics of symmetric top molecules: A comparison of the rotationally inelastic scattering of CD{sub 3} and ND{sub 3} with He". United States. https://doi.org/10.1063/1.4869596.
@article{osti_22253305,
title = {Collision dynamics of symmetric top molecules: A comparison of the rotationally inelastic scattering of CD{sub 3} and ND{sub 3} with He},
author = {Tkáč, Ondřej and Orr-Ewing, Andrew J. and Dagdigian, Paul J., E-mail: pjdagdigian@jhu.edu and Alexander, Millard H. and Onvlee, Jolijn and Avoird, Ad van der, E-mail: avda@theochem.ru.nl},
abstractNote = {We compare rotationally inelastic scattering of deuterated methyl radicals (CD{sub 3}) and ammonia (ND{sub 3}) in collisions with helium using close-coupling quantum-mechanical scattering calculations performed with ab initio potential energy surfaces (PESs). The theoretical methods have been rigorously tested against angle-resolved experimental measurements obtained using crossed molecular beam apparatuses in combination with velocity map imaging [O. Tkáč, A. G. Sage, S. J. Greaves, A. J. Orr-Ewing, P. J. Dagdigian, Q. Ma, and M. H. Alexander, Chem. Sci. 4, 4199 (2013); O. Tkáč, A. K. Saha, J. Onvlee, C.-H. Yang, G. Sarma, C. K. Bishwakarma, S. Y. T. van de Meerakker, A. van der Avoird, D. H. Parker, and A. J. Orr-Ewing, Phys. Chem. Chem. Phys. 16, 477 (2014)]. Common features of the scattering dynamics of these two symmetric top molecules, one closed-shell and the other an open-shell radical, are identified and discussed. Two types of anisotropies in the PES influence the interaction of an atom with a nonlinear polyatomic molecule. The effects of these anisotropies can be clearly seen in the state-to-state integral cross sections out of the lowest CD{sub 3} rotational levels of each nuclear spin symmetry at a collision energy of 440 cm{sup −1}. Similarities and differences in the differential cross sections for the ND{sub 3}–He and CD{sub 3}–He systems can be linked to the coupling terms derived from the PESs which govern particular initial to final rotational level transitions.},
doi = {10.1063/1.4869596},
url = {https://www.osti.gov/biblio/22253305},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 13,
volume = 140,
place = {United States},
year = {Mon Apr 07 00:00:00 EDT 2014},
month = {Mon Apr 07 00:00:00 EDT 2014}
}