I have done extensive work on the H + O2 combustion reaction in the past,
when I was in the group of dr. Evelyn Goldfield at Wayne State University.
This (endothermic) reaction,
O2 (3Σ-g) +
H (2S) --> OH (2Π) + O (3P),
is a very important reaction in combustion chemistry.
In fact, it is the rate determining step in the
combustion of hydrogen and hydrocarbons. Consequently, much experimental
and theoretical work has been done on this reaction. From a theoretical
point of view the H + O2 reaction forms a challenge for a number of reasons.
One of the most important reasons is the presence of a deep well in the
potential energy surface, corresponding to the HO2 radical, which supports
numerous bound states and gives rise to a large number of resonances. It is
therefore not surprising that rigorous quantum dynamics calculations
(for total angular momentum J=0) have only become possible in the last decade.
Given the difficulty of the problem, special care has to be taken to make
the implementation as efficient as possible. Therefore, we used parallel
computers to distribute the problem over more processors using the
``Coriolis coupled'' method of Goldfield and Gray.
This research has lead to the first-ever rigorous theoretical cross sections,
which compared well with experimental data from the Wolfrum group at the
University of Heidelberg.
We are currently applying the methods developed to the photo-dissociation
of molecules inside vanderWaals complexes, such as Ar-H2S, where angular
momentum effects allow the vanderWaals molecule to survive when one of its
constituent molecules, such as H2S, is dissociated. This work is done in
collaboration with dr. S. MacKenzie and dr. D. Hirst of Warwick University.
We also have plans to apply the developed methods to the calculation of
rates for reactions between radicals at low temperatures, which is
important for our understanding of the interstellar medium and our
understanding of extraterrestial planets and moons. This work will
be done in collaboration with Prof. I. Sims of the University of Rennes.
Some recent references
- Time-dependent quantum mechanical calculations on H + O2 for total angular momentum:
Comparing different dynamical approximations
Anthony J. H. M. Meijer and Evelyn M. Goldfield.
Phys. Chem. Chem. Phys., 3, 2811-2818 (2001).
- Dynamics of the H + O2 --> O + OH reaction: Accurate
quantum mechanical and experimental absolute reaction cross sections
Mohammed Abu Bajeh, Evelyn M. Goldfield, Alexander Hanf, Christoph
Kappel, Anthony J. H. M. Meijer, Hans-Robert Volpp, and Jürgen Wolfrum.
J. Phys. Chem. A, 105, 3359 (2001).
[PDF file on ACS web-site]
- Time-dependent quantum mechanical calculations on H + O2 for
total angular momentum J > 0 III: Total Cross sections.
Evelyn M. Goldfield and Anthony J. H. M. Meijer.
J. Chem. Phys. 113, 11055 (2000)
[gzipped PS (US-lett)].
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