Enhanced reactivity of fluorine with para-hydrogen in cold interstellar clouds by resonance-induced quantum tunnelling | |
Yang, Tiangang2; Huang, Long2,3; Xiao, Chunlei2; Chen, Jun2; Wang, Tao4; Dai, Dongxu2; Lique, Francois1,5; Alexander, Millard H.6,7; Sun, Zhigang2; Zhang, Dong H.2 | |
刊名 | NATURE CHEMISTRY |
2019-08-01 | |
卷号 | 11期号:8页码:744-749 |
ISSN号 | 1755-4330 |
DOI | 10.1038/s41557-019-0280-3 |
通讯作者 | Alexander, Millard H.(mha@umd.edu) ; Sun, Zhigang(zsun@dicp.ac.cn) ; Yang, Xueming(xmyang@dicp.ac.cn) ; Neumark, Daniel M.(dneumark@berkeley.edu) |
英文摘要 | 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. |
资助项目 | National Science Foundation of China[21688102] ; National Science Foundation of China[21590800] ; National Science Foundation of China[21127902] ; National Science Foundation of China[21433009] ; Chinese Academy of Sciences[XDB 17010000] ; Air Force Office of Scientific Research[FA9550-16-1-0097] ; US National Science Foundation[CHE-1565872] |
WOS关键词 | POTENTIAL-ENERGY SURFACE ; DYNAMICAL RESONANCES ; FESHBACH RESONANCES ; CHEMICAL-REACTIONS ; TRANSITION-STATE ; MOLECULAR-BEAM ; F+H-2 REACTION ; ATOM REACTION ; SCATTERING ; PLUS |
WOS研究方向 | Chemistry |
语种 | 英语 |
出版者 | NATURE PUBLISHING GROUP |
WOS记录号 | WOS:000476922300014 |
资助机构 | National Science Foundation of China ; National Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Air Force Office of Scientific Research ; Air Force Office of Scientific Research ; US National Science Foundation ; US National Science Foundation ; National Science Foundation of China ; National Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Air Force Office of Scientific Research ; Air Force Office of Scientific Research ; US National Science Foundation ; US National Science Foundation ; National Science Foundation of China ; National Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Air Force Office of Scientific Research ; Air Force Office of Scientific Research ; US National Science Foundation ; US National Science Foundation ; National Science Foundation of China ; National Science Foundation of China ; Chinese Academy of Sciences ; Chinese Academy of Sciences ; Air Force Office of Scientific Research ; Air Force Office of Scientific Research ; US National Science Foundation ; US National Science Foundation |
内容类型 | 期刊论文 |
源URL | [http://cas-ir.dicp.ac.cn/handle/321008/173791] |
专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
通讯作者 | Alexander, Millard H.; Sun, Zhigang; Yang, Xueming; Neumark, Daniel M. |
作者单位 | 1.Inst Univ France, Le Havre, France 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian, Liaoning, Peoples R China 3.Univ Chinese Acad Sci, Beijing, Peoples R China 4.Southern Univ Sci & Technol, Coll Sci, Dept Chem, Shenzhen, Peoples R China 5.Univ Le Havre Normandie, CNRS, Lab Ondes & Milieux Complexes, Le Havre, France 6.Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA 7.Univ Maryland, Inst Phys Sci & Technol, College Pk, MD 20742 USA 8.Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA 9.Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA |
推荐引用方式 GB/T 7714 | Yang, Tiangang,Huang, Long,Xiao, Chunlei,et al. Enhanced reactivity of fluorine with para-hydrogen in cold interstellar clouds by resonance-induced quantum tunnelling[J]. NATURE CHEMISTRY,2019,11(8):744-749. |
APA | Yang, Tiangang.,Huang, Long.,Xiao, Chunlei.,Chen, Jun.,Wang, Tao.,...&Neumark, Daniel M..(2019).Enhanced reactivity of fluorine with para-hydrogen in cold interstellar clouds by resonance-induced quantum tunnelling.NATURE CHEMISTRY,11(8),744-749. |
MLA | Yang, Tiangang,et al."Enhanced reactivity of fluorine with para-hydrogen in cold interstellar clouds by resonance-induced quantum tunnelling".NATURE CHEMISTRY 11.8(2019):744-749. |
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