期刊
NATURE CHEMISTRY
卷 7, 期 11, 页码 921-926出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2359
关键词
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资金
- European Commission through ERC [EU-FP7-ERC-CoG 1485 QuCC]
- Alexander von Humboldt Foundation
- Lee Family Foundation
- UK's Engineering and Physical Sciences Research Council through the Career Acceleration Fellowship [EP/H003657/1]
- UK's Engineering and Physical Sciences Research Council through the Programme Grant on Attosecond Dynamics [EP/I032517]
- Deutsche Forschungsgemeinschaft
- EPSRC [EP/H003657/1, EP/I032517/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/I032517/1, EP/H003657/1] Funding Source: researchfish
The role of internal molecular degrees of freedom, such as rotation, has scarcely been explored experimentally in low-energy collisions despite their significance to cold and ultracold chemistry. Particularly important to astrochemistry is the case of the most abundant molecule in interstellar space, hydrogen, for which two spin isomers have been detected, one of which exists in its rotational ground state whereas the other is rotationally excited. Here we demonstrate that quantization of molecular rotation plays a key role in cold reaction dynamics, where rotationally excited ortho-hydrogen reacts faster due to a stronger long-range attraction. We observe rotational state-dependent non-Arrhenius universal scaling laws in chemi-ionization reactions of para-H-2 and ortho-H-2 by He(2(3)P(2)), spanning three orders of magnitude in temperature. Different scaling laws serve as a sensitive gauge that enables us to directly determine the exact nature of the long-range intermolecular interactions. Our results show that the quantum state of the molecular rotor determines whether or not anisotropic long-range interactions dominate cold collisions.
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