Helium Tagging of Protonated Methane in Messenger Spectroscopy: Does It Interfere with the Fluxionality of CH5+?,Angewandte Chemie International Edition

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Helium Tagging of Protonated Methane in Messenger Spectroscopy: Does It Interfere with the Fluxionality of CH5+?
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-10-12 , DOI: 10.1002/anie.201808531
Felix Uhl ₁ , Dominik Marx ₁

Affiliation

Messenger infrared predissociation spectroscopy is an powerful technique to investigate elusive molecules. Despite accumulating evidence that ⁴He‐tagging has a minor effect on structure due to its weak interactions, its impact on intramolecular large‐amplitude motion is much less clear. Using one of the most floppy molecules known, protonated methane, we investigate to what extent helium tags perturb its salient fluxionality, underlying full hydrogen scrambling. Bosonic path integral quantum simulations show that the impact of attaching up to four ⁴He messengers to CH₅⁺ is negligible compared to the non‐tagged bare species. This non‐invasive nature is unrelated to the bosonic character of ⁴He. Yet, hydrogen scrambling has a pronounced effect on the microsolvation shell pattern of CH₅⁺⋅He_n that emerges as a result of tagging. These findings should provide impetus to explore the power of He‐tagging, particularly in the realm of weakly bound intermolecular complexes.

中文翻译：

信使光谱中质子化甲烷的氦标记：是否会干扰CH5 +的流度？

Messenger红外预离解光谱技术是研究难以捉摸的分子的强大技术。尽管有越来越多的证据表明⁴ He标记由于其弱相互作用而对结构的影响较小，但对分子内大振幅运动的影响尚不清楚。使用已知的最松散的分子之一，质子化的甲烷，我们研究了氦标记在多大程度上扰乱了其显着的通量性，而氢的扰乱是潜在的。Bosonic路径积分量子模拟表明，与未标记的裸物种相比，最多将四个⁴ He信使附接到CH ₅⁺上的影响可忽略不计。这种非侵入性与⁴的玻色特征无关他。然而，氢加扰对CH的microsolvation壳图案的显着的效果₅⁺ ⋅He _Ñ浮现作为标记的结果。这些发现应为探索He-taging的力量提供动力，尤其是在弱结合分子间复合物领域。

更新日期：2018-10-12

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