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