State-to-state Quantum Dynamics of Reaction N+NH→N2+H

doi:10.7503/cjcu20150596

Abstract

Abstract:

Quantum dynamics of reaction N+NH→N₂+H was investigated based on the recently constructed potential energy surface(PES) of N₂H(1²A') by Chebyshev real wavepacket method. The reaction probabilities, integral and diffe-rential cross sections, and ro-vibrational state distributions of the product were reported and compared with previous theoretical results. Besides, the calculated rate constants monotonically increase with the temperature from 50 K to 500 K, consistent with the available theoretical results obtained from other PESs. However, all the calculated values are significantly larger than the only experimental data at room temperature.

Key words: Quantum dynamics, Wavepacket propagation, Cross section, Rate constant

CLC Number:

O641

TrendMD:

HU Xixi, YANG Junying, XIE Daiqian. State-to-state Quantum Dynamics of Reaction N+NH→N₂+H[J]. Chem. J. Chinese Universities, 2015, 36(11): 2198.

Figures/Tables 7

Table 1 Numerical parameters(in atomic units) used in the CRWP calculations

Grid ranges and basis sizes	R∈[0.7, 17.5], $N R 1$ =499, $N R 2$ =99 r∈[1.2, 14.5], $N r 1$ =161, $N r 2$ =29 γ∈[0, 180°], j=0—j_max=100, N_j=101
Projection	$R ∞' = 9.0$
Initial wavepacket	R₀=12.5, δ=0.18, E₀=0.20 eV
Damping function	D= $exp [- 0.222 (R - 14.0 3.5) 2], 14.0 ≤ R ≤ 17.5 exp [- 0.1 (r - 13.3 1.2) 2 - 0.05], 13.3 < r ≤ 14.5 exp [- 0.05 (r - 10.8 2.5) 2], 10.8 ≤ r ≤ 13.3 1, ot h erwise$
Potential energy cutoff	7.0 eV
Rotational kinetic energy cutoff	5.0 eV
Propagation step	30000

Table 1 Numerical parameters(in atomic units) used in the CRWP calculations

Grid ranges and basis sizes	R∈[0.7, 17.5], $N R 1$ =499, $N R 2$ =99 r∈[1.2, 14.5], $N r 1$ =161, $N r 2$ =29 γ∈[0, 180°], j=0—j_max=100, N_j=101
Projection	$R ∞' = 9.0$
Initial wavepacket	R₀=12.5, δ=0.18, E₀=0.20 eV
Damping function	D= $exp [- 0.222 (R - 14.0 3.5) 2], 14.0 ≤ R ≤ 17.5 exp [- 0.1 (r - 13.3 1.2) 2 - 0.05], 13.3 < r ≤ 14.5 exp [- 0.05 (r - 10.8 2.5) 2], 10.8 ≤ r ≤ 13.3 1, ot h erwise$
Potential energy cutoff	7.0 eV
Rotational kinetic energy cutoff	5.0 eV
Propagation step	30000

Fig.1 Reaction probabilities as a function of collision energy for J=0, 30, 60, 80 and 90 eV

Fig.2 Total ICSs as a function of collision energy

Fig.3 Vibrational state distributions of N2 product at Ec=0.05, 0.10 and 0.20 eV

Fig.4 Rotational state distributions of N2 product at all vibrational levels at Ec=0.10 eV

Fig.5 Total DCSs as a function of scattering angle

Fig.6 Rate constants for the title reaction as a function of temperature

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State-to-state Quantum Dynamics of Reaction N+NH→N₂+H

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