Close-Coupling Time-Dependent Quantum Dynamics Study of the H + HCl Reaction

Yao, Li; Han, Keli; Song, He-Shan; Zhang, Donghui

doi:10.1021/jp027056v

Cited by 13 publications

(12 citation statements)

References 40 publications

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“…[22][23][24][25][26] However, concerning this method, very little has been reported for a nonreactive scattering system when two or more diabatic potential surfaces are involved. [22][23][24][25][26] However, concerning this method, very little has been reported for a nonreactive scattering system when two or more diabatic potential surfaces are involved.…”

Section: Calculation Methodsmentioning

confidence: 99%

Nonadiabatic energy transfer studies of O(1D)+N2(X 1Σg+)→O(3P)+N2(X 1Σg+) by time-dependent wave packet

Chu

Xie

Han

2004

The Journal of Chemical Physics

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Three-dimensional time-dependent quantum calculations have been performed on two/three coupled potential surfaces, including the singlet surface 1 (1)A(') and two triplet surfaces 1 (3)A(') and 1 (3)A("), for the electronic quenching process of O((1)D)+N(2)(X (1)Sigma(g) (+))-->O((3)P)+N(2)(X (1)Sigma(g) (+)). An extended split-operator scheme was employed to study this nonadiabatic process. Two types of singlet surface 1 (1)A('), namely, double many body expansion (DMBE2) were used in the calculations, along with spin-orbit couplings of Nakamura-Kato and with a constant value of 80 cm(-1). All the calculated probabilities are resonance dominated, with a general decreasing trend within the investigated collision energy range. The probability involving three potential energy surfaces is approximately two times as high as that on two potential energy surfaces. At low collision energies, the calculations on the ZPM2 surface produced much larger probability than that on the DMBE2 surface, but the difference was diminishing as the collision energy became high. The behavior of the probability on DMBE2/ZPM2 surfaces at low energies indicates that the ZPM2 surface dominates over the DMBE2 surface in the description of the process. However, the DMBE2 surface has been modified by removing the unreasonable barrier. The estimated quenching cross sections both on the ZPM2 surface and on the modified DMBE2 surface in the three-coupled-surface calculations agree with the experimental measurement. Also, a rather insensitive characteristic of the probability relative to the analytical function form of spin-orbit coupling is revealed.

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Section: Calculation Methodsmentioning

confidence: 99%

Nonadiabatic energy transfer studies of O(1D)+N2(X 1Σg+)→O(3P)+N2(X 1Σg+) by time-dependent wave packet

Chu

Xie

Han

2004

The Journal of Chemical Physics

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“…The shifting constant is determined by 32 (9) where k B is the Boltzmann constant, T is the temperature, and Q J i is a partition-like function defined as (10) where J i is a reference angular momentum which divides total angular momentum into different ranges, 32 and Q J is similarly defined as (11) where P J (E) are the probabilities for a total angular momentum quantum number from a given initial state. 39 The numerical parameters of the four reactions for the wave packet propagation are as follows: A total of 100 vibrational functions are employed for r in the range of [0.8,8.5] a 0 for the reagents HCl/DCl in the interaction region. A total number of 200 sine functions (among them 80 for the interaction region) are employed for the translational coordinate R in a range of [0.8,14.0] a0.…”

Section: + -mentioning

confidence: 99%

“…A total number of 200 sine functions (among them 80 for the interaction region) are employed for the translational coordinate R in a range of [0.8,14.0] a0. 39 For the rotational basis we use jmax = 45. The number of K used in our calculation is given by Kmax = max (3, K0+2) starting with K0 = 0.…”

Section: + -mentioning

confidence: 99%

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Theoretical Study of the X+YCl (X, Y=H, D) Reactions

Yao¹,

Han²,

Song³

et al. 2003

J Chinese Chemical Soc

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Time‐dependent wave packet calculations for the reaction H+HCl and its isotopic reactions are carried out on the potential energy surface (PES) of Bian and Werner (BW2) [Bain, W.; Werner, H.‐J. J. Chem. Phys. 2000, 112, 220]. Reaction probabilities for the exchanged and abstraction channels are calculated from various initial rotational states of the reagent. Those have then been used to estimate reaction cross sections and rate constants which also are calculated and explained by the zero‐point energy and the tunneling effect. The results of this work were compared with that of previous quasiclassical trajectory calculations and reaction dynamics experiments on the abstraction channel. In addition, the calculated rate constants are in reasonably good agreement with experimental measurements for both channels.

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“…12,13 Considerable efforts have also been made to validate the accuracy of the G3 and BW2 PESs by performing reaction dynamics calculations using quasi-classical trajectory (QCT) 17,27 or quantum methods. 28,29 On the G3 PES, Aoiz et al 30,31 carried out a QCT investigation of the pendular orientation effects in the H + DCl reaction. They concluded that rotational excitation has a minor effect on reactivity while vibrational excitation lowers the threshold and increases the cross section.…”

Section: Introductionmentioning

confidence: 99%

Time-dependent wave packet state-to-state dynamics of H/D + HCl/DCl reactions

Song

Lee

2013

The Journal of Chemical Physics

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The H/D + HCl/DCl (v(0) = 0, j(0) = 0) reactions were investigated in the gas phase using the reactant coordinate based time-dependent wave packet method on the BW2 PES [W. Bian and H.-J. Werner, J. Chem. Phys. 112, 220 (2000)]. The total and state-to-state integral and differential cross sections of both the abstraction and the exchange channels were reported over the energy range from threshold to 2.0 eV. The theoretical total exchange integral cross sections agree well with Volpp's experimental measurements but differ from Polanyi's experimental results for H + DCl reaction. The theoretical total abstraction integral cross sections are more than twice as large as the experimental results from the two groups for the H + HCl/DCl reactions. For the four isotope combinations, the total exchange integral cross sections increase monotonically with collisional energy while the abstraction integral cross sections start to decrease at relatively high collision energies. And the abstraction products are predominantly backward and sideways scattered while the exchange products are almost backward scattered. For the two channels, the D + HCl reaction presents the highest reactivity, the H + DCl reaction presents the lowest reactivity, and the H + HCl and D + DCl reactions are in between with the H + HCl reaction having a slightly larger reactivity.

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Close-Coupling Time-Dependent Quantum Dynamics Study of the H + HCl Reaction

Cited by 13 publications

References 40 publications

Nonadiabatic energy transfer studies of O(1D)+N2(X 1Σg+)→O(3P)+N2(X 1Σg+) by time-dependent wave packet

Nonadiabatic energy transfer studies of O(1D)+N2(X 1Σg+)→O(3P)+N2(X 1Σg+) by time-dependent wave packet

Theoretical Study of the X+YCl (X, Y=H, D) Reactions

Time-dependent wave packet state-to-state dynamics of H/D + HCl/DCl reactions

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