Cation, Anion, and Radical Isomers of C4H4N: Computational Characterization and Implications for Astrophysical and Planetary Environments.,The Journal of Physical Chemistry A

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Cation, Anion, and Radical Isomers of C4H4N: Computational Characterization and Implications for Astrophysical and Planetary Environments.
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-03-03 , DOI: 10.1021/acs.jpca.9b11305
Josie Hendrix ₁ , Partha P Bera _{2,

3} , Timothy J Lee ₂ , Martin Head-Gordon ₁

Affiliation

Nitrogen-containing ions and molecules in the gas phase have been detected in non-Earth environments such as dark molecular clouds and more recently in the atmosphere of Saturn's moon Titan. These molecules may serve as precursors to larger heterocyclic structures that provide the foundation of complex biological molecules. On Titan, molecules of m/z 66 have been detected by the Cassini mission, and species of the empirical formula C4H4N may contribute to this signature. We have characterized seven isomers of C4H4N in anionic, neutral radical, and cationic states using density functional theory. Structures were optimized using the range-separated hybrid ωB97X-V with the cc-pVTZ and aug-cc-pVTZ basis sets. Anionic and radical C4H4N favor cyclic structures with aromatic and quasi-aromatic electron arrangements, respectively. Interestingly, ionization from the radical surface to the cation induces significant changes in structural stability, and the global minimum for positively charged isomers is CH2CCHCNH+, a pseudo-linear species reminiscent of cyanoallene. Select formation pathways to these structures from Titan's existing or postulated gas-phase species, reactions that are also relevant for other astrophysical environments, are discussed. By characterizing C4H4N isomers, we have identified energetically stable anionic, radical, and cationic structures that may be present in Titan's atmosphere and dark molecular clouds.

中文翻译：

C4H4N的阳离子，阴离子和自由基异构体：天体物理和行星环境的计算表征及其含义。

在非地球环境中，例如黑暗的分子云中，以及最近在土星的卫星土卫六大气中，已经检测到气相中的含氮离子和分子。这些分子可以充当较大杂环结构的前体，后者为复杂的生物分子奠定了基础。在土卫六上，卡西尼号任务已检测到m / z 66的分子，经验式C4H4N的种类可能有助于此签名。我们已经使用密度泛函理论在阴离子，中性自由基和阳离子状态下表征了C4H4N的七个异构体。使用带有cc-pVTZ和aug-cc-pVTZ基础集的范围分隔的混合ωB97X-V对结构进行了优化。阴离子和自由基C4H4N分别支持具有芳族和准芳族电子排列的环状结构。有趣的是从自由基表面到阳离子的电离会引起结构稳定性的重大变化，带正电的异构体的整体最小值为CH2CCHCNH +，这是一种让人联想到氰基丙二烯的伪线性物质。讨论了从泰坦的现有或假定的气相物质中选择这些结构的形成途径，这些反应也与其他天体环境有关。通过表征C4H4N异构体，我们确定了在土卫六大气和深色分子云中可能存在的能量稳定的阴离子，自由基和阳离子结构。讨论了从泰坦的现有或假定的气相物质中选择这些结构的形成途径，这些反应也与其他天体环境有关。通过表征C4H4N异构体，我们确定了在土卫六大气和深色分子云中可能存在的能量稳定的阴离子，自由基和阳离子结构。讨论了从泰坦的现有或假定的气相物质中选择这些结构的形成途径，这些反应也与其他天体环境有关。通过表征C4H4N异构体，我们确定了在土卫六大气和深色分子云中可能存在的能量稳定的阴离子，自由基和阳离子结构。

更新日期：2020-03-03

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