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从头算研究三重态 POOH 的精细和超精细相互作用。

Ab Initio Study of Fine and Hyperfine Interactions in Triplet POH.

机构信息

Scuola Normale Superiore, Piazza dei Cavalieri 7, 56126 Pisa, Italy.

Dipartimento di Chimica "Giacomo Ciamician", Università di Bologna, Via F. Selmi 2, 40126 Bologna, Italy.

出版信息

Molecules. 2022 Jan 4;27(1):302. doi: 10.3390/molecules27010302.

Abstract

Phosphorous-containing molecules have a great relevance in prebiotic chemistry in view of the fact that phosphorous is a fundamental constituent of biomolecules, such as RNA, DNA, and ATP. Its biogenic importance has led astrochemists to investigate the possibility that P-bearing species could have formed in the interstellar medium (ISM) and subsequently been delivered to early Earth by rocky bodies. However, only two P-bearing molecules have been detected so far in the ISM, with the chemistry of interstellar phosphorous remaining poorly understood. Here, in order to shed further light on P-carriers in space, we report a theoretical spectroscopic characterisation of the rotational spectrum of POH in its 3A″ ground electronic state. State-of-the-art coupled-cluster schemes have been employed to derive rotational constants, centrifugal distortion terms, and most of the fine and hyperfine interaction parameters, while the electron spin-spin dipolar coupling has been investigated using the multi-configuration self-consistent-field method. The computed spectroscopic parameters have been used to simulate the appearance of triplet POH rotational and ro-vibrational spectra in different conditions, from cold to warm environments, either in gas-phase experiments or in molecular clouds. Finally, we point out that the predicted hyperfine structures represent a key pattern for the recognition of POH in laboratory and interstellar spectra.

摘要

含磷分子在原始化学中具有重要意义,因为磷是生物分子如 RNA、DNA 和 ATP 的基本组成部分。其生物重要性促使天体化学家研究含磷物质是否有可能在星际介质(ISM)中形成,并随后通过岩石体输送到早期地球。然而,迄今为止,在 ISM 中仅检测到两种含磷分子,星际磷的化学性质仍未得到很好的理解。为了进一步了解太空中的磷载体,我们报告了 PO* 在其 3A″ 基态电子态中的转动光谱的理论光谱特征。采用最先进的耦合簇方案来推导出转动常数、离心变形项以及大部分精细和超精细相互作用参数,而电子自旋-自旋偶极耦合则使用多组态自洽场方法进行了研究。所计算的光谱参数用于模拟不同条件下(从冷到热环境),无论是在气相实验还是在分子云中,三重态 PO* 转动和 ro-振动光谱的出现。最后,我们指出,预测的超精细结构代表了识别实验室和星际光谱中 PO* 的关键模式。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0d72/8746536/6fbcc8f2cfb8/molecules-27-00302-g001.jpg

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