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高富集对 - H3⁺ 的离解复合

Dissociative recombination of highly enriched para-H3+.

作者信息

Tom Brian A, Zhaunerchyk Vitali, Wiczer Michael B, Mills Andrew A, Crabtree Kyle N, Kaminska Magdalena, Geppert Wolf D, Hamberg Mathias, Af Ugglas Magnus, Vigren Erik, van der Zande Wim J, Larsson Mats, Thomas Richard D, McCall Benjamin J

机构信息

Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, USA.

出版信息

J Chem Phys. 2009 Jan 21;130(3):031101. doi: 10.1063/1.3065970.

Abstract

The determination of the dissociative recombination rate coefficient of H(3) (+) has had a turbulent history, but both experiment and theory have recently converged to a common value. Despite this convergence, it has not been clear if there should be a difference between the rate coefficients for ortho-H(3) (+) and para-H(3) (+). A difference has been predicted theoretically and could conceivably impact the ortho:para ratio of H(3) (+) in the diffuse interstellar medium, where H(3) (+) has been widely observed. We present the results of an experiment at the CRYRING ion storage ring in which we investigated the dissociative recombination of highly enriched ( approximately 83.6%) para-H(3) (+) using a supersonic expansion source that produced ions with T(rot) approximately 60-100 K. We observed an increase in the low energy recombination rate coefficient of the enriched para-H(3) (+) by a factor of approximately 1.25 in comparison to H(3) (+) produced from normal H(2) (ortho:para=3:1). The ratio of the rate coefficients of pure para-H(3) (+) to that of pure ortho-H(3) (+) is inferred to be approximately 2 at low collision energies; the corresponding ratio of the thermal rate coefficients is approximately 1.5 at electron temperatures from 60 to 1000 K. We conclude that this difference is unlikely to have an impact on the interstellar ortho:para ratio of H(3) (+).

摘要

H₃⁺离解复合速率系数的测定历程波折,但近期实验和理论得出了一个共同值。尽管达成了这一共识,但尚不清楚仲-H₃⁺和正-H₃⁺的速率系数是否应该存在差异。理论上预测存在差异,并且可以想象这可能会影响弥漫星际介质中H₃⁺的正仲比,在该介质中已广泛观测到H₃⁺。我们展示了在CRYRING离子储存环上进行的一项实验结果,在该实验中,我们使用产生转动温度T(rot)约为60 - 100K离子的超声速膨胀源,研究了高度富集(约83.6%)的仲-H₃⁺的离解复合。我们观察到,与由正常H₂(正仲比 = 3:1)产生的H₃⁺相比,富集仲-H₃⁺的低能复合速率系数增加了约1.25倍。在低碰撞能量下,纯仲-H₃⁺与纯正-H₃⁺的速率系数之比推断约为2;在电子温度为60至1000K时,相应的热速率系数之比约为1.5。我们得出结论,这种差异不太可能对星际介质中H₃⁺的正仲比产生影响。

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