Quantum resonances near absolute zero

doi:10.1126/science.abb8020

GSTDTAP > 气候变化

DOI	10.1126/science.abb8020
	Quantum resonances near absolute zero
	Tiangang Yang; Xueming Yang
	2020-05-08
发表期刊	Science
出版年	2020
英文摘要	Modeling atomic and molecular collisions precisely requires knowing the details of the key elementary processes that dictate their outcomes. Understanding the quantum nature of atomic and molecular collisions is essential, especially in the low–collisional energy region, where quantum effects are most prominent. Among these features are collision resonances, which are in essence transiently trapped quantum states ([ 1 ][1]–[ 3 ][2]). Their transient nature makes them inherently difficult to probe experimentally. On page 626 of this issue, de Jongh et al. ([ 4 ][3]) report a combined experimental and theoretical dynamics study on the resonances in the NO + He collision, a benchmark system for the inelastic collision energy transfer process, at very low collision energies ([ 4 ][3]). Collision resonances are attributed to quasi-bound quantum states with a, more accurate potential energy surface (PES) for NO-He. To observe these resonances, de Jongh et al. measured quantum state-to-state integral and different cross sections (event probabilities) of the inelastic NO( j = ½ f ) + He → NO( j = ½ e ) + He collision, where j is the near-degenerate doublet rotational levels f and e of the ground electronic and vibrational state of NO. These doublet states differ in symmetry, and the collision with He deexcites the slightly higher-energy upper f state to the lower-energy e state. These states were measured by using a high-resolution velocity map imaging technique in the collision energy range of 0.2 to 8.5 cm−1, corresponding to an extremely low-temperature range from 0.3 to 12.3 K. ![Figure][4] Resonance-enhanced reactivity For a high reaction barrier, rates should be almost zero at low collision energies corresponding to low temperatures. However, reaction rates can be boosted over an energy window by tunneling into a quasi-bound excited state of the products, as shown for the F + H2 reaction ([ 7 ][5]). GRAPHIC: V. ALTOUNIAN/ SCIENCE The extremely low collision energy was achieved by using the Stark decelerated molecular beam of NO( j = ½ f ) and a cryogenic He beam. It improves the study on this collision by the same group ([ 5 ][6]) and allows detailed investigation of inelastic collision dynamics in the onset regime of individual partial-wave resonances. These resonances arise from collisions with different orbital angular momentum (ℓ) partial waves, associated with the colliding molecular partners and which only a few experiments can directly access. A number of distinct peaks were observed in the state-to-state integral cross sections and assigned to quantum resonances arising from quasi-bound states on adiabatic potentials with ℓres ≥ 2. The lowest ℓres = 2 resonance observed is characterized by nearly equal contributions of outgoing partial waves with ℓout = 0 ( s -wave) and ℓout = 1 ( p -wave). Accurate quantum dynamics calculations are in excellent agreement with experimental results. Particularly interesting is that the resonances could only be accurately described with a new NO-He PES at the CCSDT(Q) level (coupled clusters singles, doubles, triples, and quadruples), demonstrating the exceptionally high level of the resonance model, characterized by both experiment and theory, for this benchmark inelastic collision system. The collision resonances are attributed to the quasi-bound quantum states on the PES. This combined experimental and theoretical study sets a standard for inelastic scattering study of atom-diatom collisions at temperatures near the absolute zero. Inelastic collision resonances are nevertheless not specific to the NO + He system; such resonances could also exist in many other inelastic collision systems at very low collision energy. In addition to inelastic scattering processes, resonances also exist in chemical reactive collisions in the low–collisional energy regime. An important benchmark for reaction resonances is the F + H2 → HF + H reaction, which is a major source of HF formation in interstellar clouds. Understanding the HF formation mechanism through this reaction at temperatures near 0 K has astrophysical implications as it can help determine hydrogen column density in space. The F + H2 reaction has a substantial reaction barrier (629 cm−1), so product formation should be negligible at low temperatures near absolute zero. However, rate measurements of the F + H2 reaction by using the CRESU technique (reaction kinetics in uniform supersonic flow) showed pronounced chemical reactivity at temperatures as low as 11 K ([ 6 ][7]). A more recent detailed crossed-beams study on this reaction in the collision energy range of 9.8 to 282 cm−1 showed that the reaction resonance peak at the energy around −40 cm−1 on the product side is responsible for the enhanced reactivity (see the figure) near 0 K ([ 7 ][5]). Because of this resonance-enhanced quantum tunneling through the reaction barrier, the rate was substantially enhanced at temperatures approaching 0 K. The quasi-bound resonance detected in the crossed-beams study was also in good agreement with the negative-ion photodetachment spectroscopic results ([ 8 ][8]). The study by de Jongh et al. is among advances made recently in the study of quantum resonances in atomic and molecular collisions at temperatures near absolute zero. Experimental breakthroughs have mainly been enabled by emerging molecular-beam methods and better detection techniques. Strong interplay between experiment and theory has also enhanced our understanding of transient resonances in collisions to a level of spectroscopic accuracy. Dynamics studies of atomic and molecular collisions are particularly important to the understanding of energy transfer and chemical reaction processes in gas-phase systems. Such studies affect the understanding of physical and chemical processes in a wide range of systems, including terrestrial and planetary atmospheres, interstellar clouds, gas-phase lasers, semiconductor processing, plasmas, and combustion processes. 1. [↵][9]1. S. Chefdeville et al ., Science 341, 1094 (2013). [OpenUrl][10][Abstract/FREE Full Text][11] 2. 1. T. Wang et al ., Chem. Soc. Rev. 47, 6744 (2018). [OpenUrl][12] 3. [↵][13]1. H. Yang et al ., Science 363, 261 (2019). [OpenUrl][14][Abstract/FREE Full Text][15] 4. [↵][16]1. T. de Jongh et al ., Science 368, 626 (2020). [OpenUrl][17][Abstract/FREE Full Text][18] 5. [↵][19]1. S. N. Vogels et al ., Science 350, 787 (2015). [OpenUrl][20][Abstract/FREE Full Text][21] 6. [↵][22]1. M. Tizniti et al ., Nat. Chem. 6, 141 (2014). [OpenUrl][23][CrossRef][24][PubMed][25] 7. [↵][26]1. T. Yang et al ., Nat. Chem. 11, 744 (2019). [OpenUrl][27] 8. [↵][28]1. J. B. Kim et al ., Science 349, 510 (2015). [OpenUrl][29][Abstract/FREE Full Text][30] Acknowledgments: X.Y. acknowledges support by National Natural Science Foundation of China (grant 21688102), Chinese Academy of Sciences (grant XDB17010000). T.Y. thanks support from Shenzhen City (grant C19543101). 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领域	气候变化 ; 资源环境
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文献类型	期刊论文
条目标识符	http://119.78.100.173/C666/handle/2XK7JSWQ/249783
专题	气候变化资源环境科学
推荐引用方式 GB/T 7714	Tiangang Yang,Xueming Yang. Quantum resonances near absolute zero[J]. Science,2020.
APA	Tiangang Yang,&Xueming Yang.(2020).Quantum resonances near absolute zero.Science.
MLA	Tiangang Yang,et al."Quantum resonances near absolute zero".Science (2020).