Chemical reactions are important in the evolution of low-temperature interstellar clouds, where the quantum tunnelling effect becomes significant. The F + para-H2 → HF + H reaction, which has a significant barrier of 1.8 kcal mol−1, is an important source of HF in interstellar clouds; however, the dynamics of this quantum-tunnelling-induced reactivity at low temperature is unknown. Here, we show that this quantum tunnelling is caused by a post-barrier resonance state. Quantum-state-resolved crossed-beam scattering measurements reveal that this resonance state has a collision energy of ~5 meV and a lifetime of ~80 fs, which are in excellent agreement with a recent anion photoelectron spectroscopic study. Accurate quantum reactive scattering calculations on the new iCSZ-LWAL potential energy surfaces provides a detailed explanation of the experimental results. The reaction rate for this system was also theoretically determined accurately at temperatures as low as 1 K.
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Data supporting the findings of this study are available from the corresponding authors on request.
The accurate iCSZ and iCSZ-LWAL PESs developed in this work are available from the corresponding authors on request.
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C.X., Z.S., D.H.Z. and X.Y. acknowledge financial support for this research from the National Science Foundation of China (grants 21688102, 21590800, 21127902 and 21433009) and the Chinese Academy of Sciences (grants XDB 17010000). D.M.N. thanks the Air Force Office of Scientific Research for funding this research under grant no. FA9550-16-1-0097. M.H.A. thanks the US National Science Foundation for support under grant no. CHE-1565872.
The authors declare no competing interests.
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Supplementary Figs. 1–9, Supplementary Tables 1 and 2, Supplementary methods
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Physics of Life Reviews (2019)