Seven-degree-of-freedom, quantum scattering dynamics study of the H{sub 2}D{sup +}+H{sub 2} reaction

Journal Article · Sun Feb 28 04:00:00 EST 2010 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.3329730· OSTI ID:21559837

Dunyou, Wang ^[1]; Zhen, Xie; Bowman, Joel M ^[2]

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1. College of Physics and Electronics, Shandong Normal University, Jinan, Shandong 250014 (China)
2. Department of Chemistry and Cherry L. Emerson Center of Scientific Computation, Emory University, Atlanta, Georgia 30322 (United States)

A quantum scattering dynamics, time-dependent wavepacket propagation method is applied to study the reaction of H{sub 2}D{sup +}+H{sub 2}{yields}H{sub 3}{sup +}+HD on the Xie-Braams-Bowman potential energy surface. The reduced-dimensional, seven-degree-of-freedom approach is employed in this calculation by fixing one Jacobi and one torsion angle related to H{sub 2}D{sup +} at the lowest saddle point geometry of D{sub 2d} on the potential energy surface. Initial state selected reaction probabilities are presented for various initial rovibrational states. The ground state reaction probability shows no threshold for this reaction, in other words, this reaction can occur without an activation barrier. The vibrational excitation shows that the stretching motion of H{sup +}-HD only has a small effect on the reaction probability; the vibrational excitation of HD in H{sub 2}D{sup +} hinders the reactivity. By contrast, rotational excitation of H{sup +}-HD greatly enhances the reactivity with the reaction probability increased double or triple at high rotational states compared to the ground state. Reactive resonances, seen in all the initial state selected reaction probabilities, are also found in the integral cross section for the ground state of H{sub 2}D{sup +} and H{sub 2}. The thermal rate coefficient is also calculated and is found to be in semiquantitative agreement with experiment; however, quantum scattering approaches including more degrees of freedom, especially including all the angles, are necessary to study this reaction in the future.

• OSTI ID: 21559837
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 8 Vol. 132; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
74 ATOMIC AND MOLECULAR PHYSICS
COLLISIONS
CROSS SECTIONS
DEGREES OF FREEDOM
ELEMENTS
ENERGY
ENERGY LEVELS
ENERGY-LEVEL TRANSITIONS
EXCITATION
EXCITED STATES
GROUND STATES
HYDROGEN
HYDROGEN COMPOUNDS
INTEGRAL CROSS SECTIONS
ION COLLISIONS
ION-MOLECULE COLLISIONS
ISOTOPES
MOLECULE COLLISIONS
MOLECULES
NONMETALS
POTENTIAL ENERGY
PROBABILITY
REACTIVITY
RESONANCE
ROTATIONAL STATES
SCATTERING
SURFACES
TIME DEPENDENCE
VIBRATIONAL STATES
WAVE PACKETS