Roles Of Large Amplitude Motions In The Dynamics Of The Proton Transfer Reaction H3+ + H2→ H5+→ H3+ + H2

Lin, Zhou

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https://hdl.handle.net/2142/51082 Copy

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Title

Roles Of Large Amplitude Motions In The Dynamics Of The Proton Transfer Reaction H3+ + H2→ H5+→ H3+ + H2

Author(s)

Lin, Zhou

Contributor(s)

McCoy, Anne B.

Issue Date

2014-06-16

Keyword(s)

Mini-symposium: Spectroscopy in Kinetics and Dynamics

Abstract

H$_3^+$ $+$ H$_2\rightarrow$ H$_5^+\rightarrow$ H$_3^+$ $+$ H$_2$ is a prototypical proton transfer reaction of astrochemical significance. Developing a deeper understanding of its reaction mechanism will provide important physical insights into similar and more complicated proton transfer reactions. The large amplitude vibrational motions in the H$_5^+$ collision complex lead to the scrambling of its five protons, which complicates theoretical descriptions of this molecular ion. Using minimized energy path diffusion Monte Carlo, the one-dimensional zero-point corrected potential energy surface is mapped out as a function of the chosen reaction coordinate.{\footnote{C. E. Hinkle and A. B. McCoy, J. Phys. Chem. Lett., 1, 562 (2010)}} The evolution of the wave function along this reaction coordinate is characterized by the energy and the probability amplitude associated to it. This methodology is also extended to allow for the investigation of excited states in selected vibrational modes that are important in the proton scrambling dynamics. In particular, the vibrations of interest are ones that evolve between large amplitude motions in H$_5^+$ and rotations of the H$_3^+$ and H$_2$ fragments as the reaction proceeds. In addition, as H$_5^+$ has five protons we must account for the anti-symmetry of the total nuclear wave function, which places restrictions to the possible pathways involved in the proton scrambling dynamics.{\footnote{M. Quack, Mol. Phys., 34, 477 (1977)}} The implications of these symmetry restrictions are also discussed.

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

text

Language

English

Permalink

http://hdl.handle.net/2142/51082

DOI

https://doi.org/10.15278/isms.2014.MH03

Copyright and License Information

Copyright 2014 by the authors. Licensed under a Creative Commons Attribution 4.0 International License. http://creativecommons.org/licenses/by/4.0/

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