A Kinetic Study of the N(2D) + C2H4 Reaction at Low Temperature


lN(2d) as a function of the delay between photolysis and probe lasers recorded at 127 K. (Solid red circles) without C2H4; (solid blue squares) [C2H4] = 5.1 × 1014 cm-3 . [NO] = 4.7 × 1014 cm-3 for both decays. Single exponential fits to the data according to expression (3) are represented by solid red and blue lines.

Electronically excited nitrogen atoms N(2D) are important species in the photochemistry of N2 based planetary atmospheres such as Titan. Despite this, few N(2D) reactions have been studied over the appropriate low temperature range.

During the present work, rate constants were measured for the N(2D) + ethene (C2H4) reaction using a supersonic flow reactor at temperatures between 50 K and 296 K. Here, a chemical reaction was used to generate N(2D) atoms, which were detected directly by laser induced fluorescence in the vacuum ultraviolet wavelength region. The measured rate constants displayed very little variation as a function of temperature, with substantially larger values than those obtained in previous work. Indeed, considering an average temperature of 170 K for the atmosphere of Titan leads to a rate constant that is almost seven times larger than the currently recommended value.

In parallel, electronic structure calculations were performed to provide insight into the reactive process. While earlier theoretical work at a lower level predicted the presence of a barrier for the N(2D) + C2H4 reaction, the present calculations demonstrate that two of the five doublet potential energy surfaces correlating with reagents are likely to be attractive, presenting no barriers for the perpendicular approach of the N atom to the carbon double bond of ethene. The measured rate constants and new product channels taken from recent dynamical investigations of this process are included in a 1D coupled ion-neutral model of Titans atmosphere. These simulations indicate that the modeled abundances of numerous nitrogen bearing compounds are noticeably affected by these changes.

Kevin M. Hickson, Cédric Bray, Jean-Christophe Loison, Michel Dobrijevic

Comments: 21 pages, 5 figures, 2 tables
Subjects: Chemical Physics (physics.chem-ph); Earth and Planetary Astrophysics (astro-ph.EP); Atomic Physics (physics.atom-ph)
Journal reference: Phys Chem Chem Phys, 2020, 22, 14026-14035
DOI: 10.1039/d0cp02083d
Cite as: arXiv:2012.00655 [physics.chem-ph] (or arXiv:2012.00655v1 [physics.chem-ph] for this version)
Submission history
From: Kevin Hickson
[v1] Tue, 10 Nov 2020 09:18:14 UTC (631 KB)
https://arxiv.org/abs/2012.00655
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