Enhanced reactivity of fluorine with para-hydrogen in cold interstellar clouds by resonance-induced quantum tunnelling

Yang, Tiangang1; Huang, Long1,2; Xiao, Chunlei1; Chen, Jun1; Wang, Tao3; Dai, Dongxu1; Lique, Francois4,5; Alexander, Millard H.6,7; Sun, Zhigang1; Zhang, Dong H.1; Yang, Xueming1,3; Neumark, Daniel M.8,9

2019-08

10.1038/s41557-019-0280-3

Nature Chemistry   影响因子和分区

1755-4330

1755-4349

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.

SCI

英语

NI论文

通讯

US National Science Foundation[CHE-1565872]

Chemistry

Chemistry, Multidisciplinary

WOS:000476922300014

NATURE PUBLISHING GROUP

Web of Science

1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian, Liaoning, Peoples R China
2.Univ Chinese Acad Sci, Beijing, Peoples R China
3.Southern Univ Sci & Technol, Coll Sci, Dept Chem, Shenzhen, Peoples R China
4.Univ Le Havre Normandie, CNRS, Lab Ondes & Milieux Complexes, Le Havre, France
5.Inst Univ France, 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

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.

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.

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.