Nonadiabatic quantum dynamics of C(1 D )+H2→CH+H: Coupled-channel calculations including Renner-Teller and Coriolis terms - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Chemical Physics Année : 2011

Nonadiabatic quantum dynamics of C(1 D )+H2→CH+H: Coupled-channel calculations including Renner-Teller and Coriolis terms

Paolo Defazio
  • Fonction : Auteur
Béatrice Bussery-Honvault
  • Fonction : Auteur
Pascal Honvault
Carlo Petrongolo
  • Fonction : Auteur

Résumé

The Renner-Teller (RT) coupled-channel dynamics for the ${\rm C}( {{}^1D} )+{\rm H}_{\rm 2} ( {X{}^{\rm 1}{\rm \Sigma }_g^ + } ) \to {\rm CH}( {X^2 \Pi } )\break + {\rm H}( {{}^2S} )$C(D1)+H2(XΣg+1)→ CH (X2Π)+H(S2) reaction has been investigated for the first time, considering the first two singlet states $\tilde a{}^1A^{\rm \prime }$ã1A′ and $\tilde b{}^1A^{\prime \prime }$b̃1A′′ of CH2 dissociating into the products and RT couplings, evaluated through the ab initio matrix elements of the electronic angular momentum. We have obtained initial-state-resolved probabilities, cross sections and thermal rate constants via the real wavepacket method for both coupled electronic states. In contrast to the ${\rm N}( {{}^2D} ) + {\rm H}_{\rm 2} ( {X{}^{\rm 1}{\rm \Sigma }_g^ + } )$N(D2)+H2(XΣg+1) system, RT effects tend to reduce probabilities, cross sections, and rate constants in the low energy range compared to Born-Oppenheimer (BO) ones, due to the presence of a repulsive RT barrier in the effective potentials and to long-lived resonances. Furthermore, contrary to BO results, the rate constants have a positive temperature dependence in the 100–400 K range. The two-state RT rate constant at 300 K, lower than the BO one, remains inside the error bars of the experimental value.
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hal-04465695 , version 1 (19-02-2024)

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Paolo Defazio, Béatrice Bussery-Honvault, Pascal Honvault, Carlo Petrongolo. Nonadiabatic quantum dynamics of C(1 D )+H2→CH+H: Coupled-channel calculations including Renner-Teller and Coriolis terms. Journal of Chemical Physics, 2011, 135 (11), ⟨10.1063/1.3636083⟩. ⟨hal-04465695⟩

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