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Characterization and photochemistry of XCO2 (X = F, NH2, CH3) radicals

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Abstract

The XCO2 (X = F, NH2, CH3) radicals are present in the Earth atmosphere, where they are produced by the degradation of Volatile Organic Compounds (VOCs), either industrial or natural. Here, we use advanced ab initio methodologies to characterize these species in their ground and electronically excited states. Computations are carried out using the Coupled Clusters, both standard and explicitly correlated versions, and multiconfigurational approaches. Several basis sets were used. Afterward, the geometrical parameters and the total energies were extrapolated to the complete basis set (CBS) limit. We also mapped their potentials along the central bond to have insights on the XCO2 → X + CO2 reactions. We thus show that the ground and the lowest electronic excited states are long-lived, for which we provide a set of accurate structural and spectroscopic parameters. The upper electronic states are subject of unimolecular decompositions producing CO2 and X fragments. Our calculations show that the FCO2 (X2B2) → F(2P) + CO2 (X1Σg+) and the CH3CO2 (X2A″) → CH3(X2A″2) + CO2 (X1Σg+) processes require at least 3.5 eV energy to occur, while less energy (of  ∼ 2.5 eV) is needed for the NH2CO2 (X2A″) → NH2(X2B1) + CO2 (X1Σg+) reaction. The present findings and data are useful to characterize these radicals in the laboratory, in planetary atmospheres and in combustion and to understand their physical chemistry there.

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Acknowledgements

The authors thank the Programme National “Physique et Chimie du Milieu Interstellaire” (PCMI) of Centre National de la Recherche Scientifique (CNRS)/Institut National des Sciences de l’Univers (INSU) with Institut de Chimie (INC)/Institut de Physique (INP) co-funded by Commissariat à l’Energie Atomique (CEA) and Centre National d’Etudes Spatiales (CNES). S.K. thanks a fellowship from the Tunisian ministry for higher education and research. This article is based upon work from COST Action CA18212—Molecular Dynamics in the GAS phase (MD-GAS), supported by COST (European Cooperation in Science and Technology, www.cost.eu). This work was supported by a STSM Grant to S.K. from COST Action CA18212.

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  1. Laboratoire de Spectroscopie Atomique, Moléculaire et Applications—LSAMA, Université de Tunis-El Manar, Tunis, Tunisia

    S. Kechoindi, S. Ben Yaghlane & N. Terzi

  2. Université Gustave Eiffel, COSYS/IMSE, 5 Bd Descartes, 77454, Champs Sur Marne, France

    S. Kechoindi & M. Hochlaf

  3. Sorbonne Université, CNRS, Laboratoire de Chimie Physique—Matière et Rayonnement, LCP-MR, 75005, Paris, France

    J. Palaudoux

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All authors contributed to the study conception and design. Data collection and analysis were performed by all authors. The first draft of the manuscript was written by MH and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Kechoindi, S., Ben Yaghlane, S., Terzi, N. et al. Characterization and photochemistry of XCO2 (X = F, NH2, CH3) radicals. Eur. Phys. J. Spec. Top. 232, 1905–1916 (2023). https://doi.org/10.1140/epjs/s11734-023-00918-1

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