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Formation of Highly Rovibrationally Excited Ammonia from Dissociative Recombination of NH4+

Journal article
Authors Patrik U Andersson
Jenny Öjekull
Jan B. C. Pettersson
Nikola Markovic
F. Hellberg
R.D. Thomas
A. Ehlerding
F. Osterdahl
Vitali Zhaunerchyk
W. Geppert
M. af Ugglas
M. Larsson
E. Uggerud
H. Danared
A. Källberg
Published in The Journal of Physical Chemistry Letters
Volume 1
Issue 17
Pages 2519–2523
ISSN 1948-7185
Publication year 2010
Published at Department of Chemistry
Pages 2519–2523
Language en
Links dx.doi.org/10.1021/jz100828u
Keywords dissociative recombination; ammonia; ammonium ion; storage ring; imaging technique; internal energy; direct dynamics
Subject categories Physical Chemistry

Abstract

The internal energy distribution of ammonia formed in the dissociative recombination (DR) of NH4+ with electrons has been studied by an imaging technique at the ion storage ring CRYRING. The DR process resulted in the formation of NH3 + H (0.90 ± 0.01), with minor contributions from channels producing NH2 + H2 (0.05 ± 0.01) and NH2 + 2H (0.04 ± 0.02). The formed NH3 molecules were highly internally excited, with a mean rovibrational energy of 3.3 ± 0.4 eV, which corresponds to 70% of the energy released in the neutralization process. The internal energy distribution was semiquantitatively reproduced by ab initio direct dynamics simulations, and the calculations suggested that the NH3 molecules are highly vibrationally excited while rotational excitation is limited. The high internal excitation and the translational energy of NH3 and H will influence their subsequent reactivity, an aspect that should be taken into account when developing detailed models of the interstellar medium and ammonia-containing plasmas.

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