Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate

Andersson S, Nyman G, Arnaldsson A, Manthe U, Jonsson H (2009)
Journal of Physical Chemistry A 113(16): 4468-4478.

Zeitschriftenaufsatz | Veröffentlicht | Englisch
 
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Abstract / Bemerkung
Thermal rate constants are calculated for the H + CH4 -> CH3 + H-2 reaction employing the potential energy surface of Espinosa-Garcia (Espinosa-Garcia, J. J. Chem. Phys. 2002, 116, 10664). Two theoretical approaches are used. First, we employ the multiconfigurational time-dependent Hartree method combined with flux correlation functions. In this way rate constants in the range 225-400 K are obtained and compared with previous results using the same theoretical method but the potential energy surface of Wu et al. (Wu, T.; Werner, H.-J.; Manthe, U. Science 2004, 306, 2227). It is found that the Espinosa-Garcia surface results in larger rate constants. Second, a harmonic quantum transition state theory (HQTST) implementation of instanton theory is used to obtain rate constants in a temperature interval from 20 K up to the crossover temperature at 296 K. The HQTST estimates are larger than MCTDH ones by a factor of about three in the common temperature range. Comparison is also made with various tunneling corrections to transition state theory and quantum instanton theory.
Stichworte
MULTIDIMENSIONAL TUNNELING CONTRIBUTIONS THERMAL RATE CONSTANTS EXTENDED TEMPERATURE INTERVAL HYDROGEN ABSTRACTION REACTION DEPENDENT HARTREE APPROACH FINDING SADDLE-POINTS ROTOR TARGET MODEL REDUCED-DIMENSIONALITY CHEMICAL-REACTIONS REACTIVE SCATTERING
Erscheinungsjahr
2009
Zeitschriftentitel
Journal of Physical Chemistry A
Band
113
Ausgabe
16
Seite(n)
4468-4478
ISSN
1089-5639
eISSN
1520-5215
Page URI
https://pub.uni-bielefeld.de/record/1896999

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Andersson S, Nyman G, Arnaldsson A, Manthe U, Jonsson H. Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate. Journal of Physical Chemistry A. 2009;113(16):4468-4478.
Andersson, S., Nyman, G., Arnaldsson, A., Manthe, U., & Jonsson, H. (2009). Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate. Journal of Physical Chemistry A, 113(16), 4468-4478. doi:10.1021/jp811070w
Andersson, S., Nyman, G., Arnaldsson, A., Manthe, U., and Jonsson, H. (2009). Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate. Journal of Physical Chemistry A 113, 4468-4478.
Andersson, S., et al., 2009. Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate. Journal of Physical Chemistry A, 113(16), p 4468-4478.
S. Andersson, et al., “Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate”, Journal of Physical Chemistry A, vol. 113, 2009, pp. 4468-4478.
Andersson, S., Nyman, G., Arnaldsson, A., Manthe, U., Jonsson, H.: Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate. Journal of Physical Chemistry A. 113, 4468-4478 (2009).
Andersson, Stefan, Nyman, Gunnar, Arnaldsson, Andri, Manthe, Uwe, and Jonsson, Hannes. “Comparison of Quantum Dynamics and Quantum Transition State Theory Estimates of the H+CH4 Reaction Rate”. Journal of Physical Chemistry A 113.16 (2009): 4468-4478.

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