Mutual neutralization of C$_{60}^+$ and C$_{60}^-$ ions: Excitation energies and state-selective rate coefficients

Michael Gatchell, Raka Paul, MingChao Ji, Stefan Rosén, Richard D. Thomas, Henrik Cederquist, Henning T. Schmidt, Åsa Larson, Henning Zettergren
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Abstract

Context: Mutual neutralization between cations and anions play an important role in determining the charge-balance in certain astrophysical environments. However, empirical data for such reactions involving complex molecular species has been lacking due to challenges in performing experimental studies, leaving the astronomical community to rely on decades old models with large uncertainties for describing these processes in the interstellar medium. Aims: To investigate the mutual neutralization (MN) reaction, C$_{60}^+$ + C$_{60}^-$ $\rightarrow$ C$_{60}^*$ + C$_{60}$, for collisions at interstellar-like conditions. Methods: The mutual neutralization reaction between C$_{60}^+$ and C$_{60}^-$ at collision energies of 100\,meV was studied using the Double ElectroStatic Ion Ring ExpEriment, DESIREE, and its merged-beam capabilities. To aid in the interpretation of the experimental results, semi-classical modeling based on the Landau-Zener approach was performed for the studied reaction. Results: We experimentally identify a narrow range of kinetic energies for the neutral reaction products. Modeling was used to calculate the quantum state-selective reaction probabilities, absolute cross sections, and rate coefficients of these MN reactions, using the experimental results as a benchmark. The MN cross sections are compared with model results for electron attachment to C$_{60}$ and electron recombination with C$_{60}^+$. Conclusions: The present results show that it is crucial to take mutual polarization effects, the finite sizes, and the final quantum states of both molecular ions into account for reliable predictions of MN rates expected to strongly influence the charge-balance and chemistry in, e.g., dense molecular clouds.
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C$_{60}^+$ 和 C$_{60}^-$ 离子的相互中和:激发能量和状态选择性速率系数
背景:然而,由于实验研究方面的挑战,涉及复杂分子物种的此类反应一直缺乏经验数据,使得天文学界只能依赖已有几十年历史的、具有很大不确定性的模型来描述星际介质中的这些过程。目的:研究在类星际条件下碰撞的相互中和(MN)反应:C$_{60}^+$ + C$_{60}^-$$\rightarrow$ C$_{60}^*$ + C$_{60}$。方法:为了帮助解释实验结果,对所研究的反应进行了基于朗道-齐纳方法的半经典模拟。结果:我们通过实验确定了中性反应产物的动力学能量的狭窄范围。以实验结果为基准,通过建模计算了这些中性反应的量子态选择性反应概率、绝对截面和速率系数。将 MN 截面与电子附着到 C$_{60}$ 和电子与 C$_{60}^+$ 重组的模型结果进行了比较。结论:本研究结果表明,要可靠地预测 MN 的速率,必须考虑到相互极化效应、有限尺寸以及两种分子离子的最终量子态,这些因素预计会对电荷平衡和稠密分子云等中的化学反应产生强烈影响。
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