期刊
NATURE CHEMISTRY
卷 11, 期 8, 页码 744-749出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-019-0280-3
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资金
- National Science Foundation of China [21688102, 21590800, 21127902, 21433009]
- Chinese Academy of Sciences [XDB 17010000]
- Air Force Office of Scientific Research [FA9550-16-1-0097]
- US National Science Foundation [CHE-1565872]
Chemical reactions are important in the evolution of low-temperature interstellar clouds, where the quantum tunnelling effect becomes significant. The F + para-H-2 -> 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 similar to 5 meV and a lifetime of similar to 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 1K.
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