Quasiclassical trajectory study of the C + NO reaction on a new potential energy surface

Simonson, Margaret; Markovíc, Nikola; Nordholm, Sture; Persson, B. Joakim

doi:10.1016/0301-0104(95)00236-h

Cited by 22 publications

(20 citation statements)

References 32 publications

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“…We include 167 chemical reactions, consisting of 27 exchange and 140 dissociation/recombination reactions. More information on the thermodynamic and reaction databases used for these calculations is available in the supporting information for this work (Atakan et al, 1989;Hash et al, 1994;Hassan & Hash, 1993;Ivanov et al, 1998;Park, 1990;Simonson et al, 1995;Sims & Smith, 1988;Smith et al, 1999;Tsang & Herron, 1991;Wagner & Bair, 1986;Zahnle, 1986).…”

Section: Atmospheric Chemistrymentioning

confidence: 99%

HCN Production via Impact Ejecta Reentry During the Late Heavy Bombardment

et al. 2018

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Major impact events have shaped the Earth as we know it. The Late Heavy Bombardment is of particular interest because it immediately precedes the first evidence of life. The reentry of impact ejecta creates numerous chemical by‐products, including biotic precursors such as HCN. This work examines the production of HCN during the Late Heavy Bombardment in more detail. We stochastically simulate the range of impacts on the early Earth and use models developed from existing studies to predict the corresponding ejecta properties. Using multiphase flow methods and finite‐rate equilibrium chemistry, we then find the HCN production due to the resulting atmospheric heating. We use Direct Simulation Monte Carlo to develop a correction factor to account for increased yields due to thermochemical nonequilibrium. We then model 1‐D atmospheric turbulent diffusion to find the time accurate transport of HCN to lower altitudes and ultimately surface water. Existing works estimate the necessary HCN molarity threshold to promote polymerization that is 0.01 M. For a mixing depth of 100 m, we find that the Late Heavy Bombardment will produce at least one impact event above this threshold with probability 24.1% for an oxidized atmosphere and 56.3% for a partially reduced atmosphere. For a mixing depth of 10 m, the probability is 79.5% for an oxidized atmosphere and 96.9% for a partially reduced atmosphere. Therefore, Late Heavy Bombardment impact ejecta is likely an HCN source sufficient for polymerization in shallow bodies of water, particularly if the atmosphere were in a partially reduced state.

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Section: Atmospheric Chemistrymentioning

confidence: 99%

HCN Production via Impact Ejecta Reentry During the Late Heavy Bombardment

et al. 2018

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“…12 Several theoretical investigations have been carried out later on the 2 A surface to investigate the the ro-vibrational distribution of CN at both the collision energies. [13][14][15][16][17] The ro-vibrational distribution of CN was best described when the 4 A electronic state was adiabatically included in the dynamical simulations. 17…”

Section: Introductionmentioning

confidence: 99%

“…18,19 A LEPS-type potential energy surface (PES) for 2 A symmetry of the [CNO] system has been constructed 13 followed by a many body expansion fit of the 2 A surface from CASPT2 energies. 15 This was further improved by including more ab initio energies for nonlinear geometries and analytically describing the long-range part. 20 In subsequent work, the PESs for the 2 A and 4 A symmetries of [CNO] using CASPT2 calculations and the same parametrization of the PES were constructed.…”

Section: Introductionmentioning

confidence: 99%

The C(3P) + NO(X2Π) → O(3P) + CN(X2Σ+), N(2D)/N(4S) + CO(X1Σ+) reaction: Rates, branching ratios, and final states from 15 K to 20 000 K

Koner

Bemish

Meuwly

2018

The Journal of Chemical Physics

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The C + NO collision system is of interest in the area of high-temperature combustion and atmospheric chemistry. In this work, full dimensional potential energy surfaces for the A',A″, and A″ electronic states of the [CNO] system have been constructed following a reproducing kernel Hilbert space approach. For this purpose, more than 50 000 energies are calculated at the MRCI+Q/aug-cc-pVTZ level of theory. The dynamical simulations for the C(P) + NO(XΠ) → O(P) + CN(XΣ), N(D)/N(S) + CO(XΣ) reactive collisions are carried out on the newly generated surfaces using the quasiclassical trajectory (QCT) calculation method to obtain reaction probabilities, rate coefficients, and the distribution of product states. Preliminary quantum calculations are also carried out on the surfaces to obtain the reaction probabilities and compared with QCT results. The effect of nonadiabatic transitions on the dynamics for this title reaction is explored within the Landau-Zener framework. QCT simulations have been performed to simulate molecular beam experiment for the title reaction at 0.06 and 0.23 eV of relative collision energies. Results obtained from theoretical calculations are in good agreement with the available experimental as well as theoretical data reported in the literature. Finally, the reaction is studied at temperatures that are not practically achievable in the laboratory environment to provide insight into the reaction dynamics at temperatures relevant to hypersonic flight.

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“…[31][32][33][34] Subsequent investigations include a collinear quantum wave packet calculation 35 to analyze the influence of the topology of the potential well on the collinear dynamics, a statistical study 36 to simulate the energy partitioning and rovibrational distribution of the CN molecule in crossed molecular beam experiments, and an estimation of the total rate coefficient 37 using a capture approach based upon the long-range part of the potential and including spin-orbit coupling. A more accurate PES was calculated by Persson et al, 38 which was followed by a rovibrational spectral analysis 39 of the linear triatomic molecules ͑CNO, CON, and NCO͒ and another ab initio calculation by Simonson et al 40 Most recent studies include a two-degree-of-freedom geometrical investigation 41 involving periodic orbits for the collinear CNO dynamics, a quasiclassical trajectory calculation 42 over a wide temperature range, and a three-dimensional time-dependent wavepacket study 43 for total angular momentum Jϭ0.…”

Section: Introductionmentioning

confidence: 99%

A quantum and semiclassical study of dynamical resonances in the C+NO→CN+O reaction

Abrol

Wiesenfeld

Lambert

et al. 2001

The Journal of Chemical Physics

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Accurate quantum mechanical reactive scattering calculations were performed for the collinear CϩNO→CNϩO reaction using a polynomial-modified London Eyring Polanyi Sato ͑PQLEPS͒ potential energy surface ͑PES͒, which has a 4.26 eV deep well in the strong interaction region, and a reference LEPS PES, which has no well in that region. The reaction probabilities obtained for both PESs show signatures for resonances. These resonances were characterized by calculating the eigenvalues and eigenvectors of the collision lifetime matrix as a function of energy. Many resonances were found for scattering on both PESs, indicating that the potential well in the PQLEPS PES does not play the sole role in producing resonances in this relatively heavy atom system and that Feshbach processes occur for both PESs. However, the well in the PQLEPS PES is responsible for the differences in the energies, lifetimes, and compositions of the corresponding resonance states. These resonances are also interpreted in terms of simple periodic orbits supported by both PESs ͑using the WKB formalism͒, to further illustrate the role played by that potential well on the dynamics of this reaction. The existence of the resonances is associated with the dynamics of the long-lived CNO complex, which is much different than that of systems having an activation barrier. Although these results were obtained for a collinear model of the reaction, its collinearly-dominated nature suggests that related resonant behavior may occur in the real world.

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Quasiclassical trajectory study of the C + NO reaction on a new potential energy surface

Cited by 22 publications

References 32 publications

HCN Production via Impact Ejecta Reentry During the Late Heavy Bombardment

HCN Production via Impact Ejecta Reentry During the Late Heavy Bombardment

The C(3P) + NO(X2Π) → O(3P) + CN(X2Σ+), N(2D)/N(4S) + CO(X1Σ+) reaction: Rates, branching ratios, and final states from 15 K to 20 000 K

A quantum and semiclassical study of dynamical resonances in the C+NO→CN+O reaction

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