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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Inverted Vibrational and Rotational Excitation of CN(B-2 Sigma(+)) Produced through Superexcited Ion-Pair States of MCN (M = Na, K, Rb)
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Inverted Vibrational and Rotational Excitation of CN(B-2 Sigma(+)) Produced through Superexcited Ion-Pair States of MCN (M = Na, K, Rb)

机译：通过超脆离子对MCN（M = Na，K，Rb）产生的CN（B-2 Sigma（+））的倒置振动和旋转激发

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摘要

This paper reports an energy-partition mechanism in dissociative excitation of alkali cyanide molecules, MCN (M = Rb, K, Na), to produce CN(B-2 Sigma(+)) and M(ns(2)S) (n = 5, 4, and 3 for Rb, K, and Na, respectively) in collision with Kr metastable atoms, Kr-m(3P(2,0)). Both the vibrational and rotational distributions of CN(B2 Sigma+) produced in the reactions of RbCN and KCN were inverted as being peaked at v' = 1 and N' = 35, respectively, where v' and N' are the vibrational and the rotational quantum numbers of CN(B-2 Sigma(+)), respectively. According to a state crossing model, it was derived that CN(B(2)v(+)) is produced by predissociation through a superexcited ion-pair state, CN-(3(1)Sigma(+))center dot M+(1S), followed by an adiabatic transition to a repulsive state correlating to the dissociation limit of CN(B-2 Sigma(+)) + M(ns(2)S). The inverted distributions are driven by structural changes during the excitation and the adiabatic transition. The maximum vibrational population at v' = 1 originates from a large Franck-Condon overlap between the vibrational wavefunctions of CN-(3(1 Sigma+)) and CN(B2 Sigma+) at v' = 1. The rotational excitation of the CN(B-2 Sigma(+)) product is explained with changing from a T-shape geometry of MCN in the ground state to a linear one in the superexcited ion-pair state.
机译：本文报告了碱氰化物分子分离激发的能量分配机制，MCN（M = RB，K，NA），以产生CN（B-2σ（+））和M（NS（2））（n = 5,4和3的RB，K和Na，分别为碰撞与KR亚稳态原子，KR-M（3p（2,0））。在RBCN和KCN的反应中产生的CN（B2 sigma +）的振动和旋转分布在V'= 1和N'= 35处被反转，其中V'和N'是振动和旋转分别为CN（B-2 Sigma（+））量子数。根据状态交叉模型，得出的是，通过通过超脆离子对状态，CN-（3（1）Sigma（+））中心点M +（ 1S），然后是与CN（B-2 Sigma（+））+ M（NS（2））的解离极限相关的排斥状态的绝热过渡。倒置分布是在激发过程中的结构变化和绝热转变时的驱动。 V'= 1的最大振动群来自CN-（3（1sigma +））和CN（B2 sigma +）的振动波发生器之间的大的Franck-Condon重叠在V'= 1. CN的旋转激励（ B-2 Sigma（+））通过从接地状态的MCN的T形几何形状改变为基于超脆离子对状态的线性索引。

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