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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Collision-partner dependence of energy transfer between the CH A(2)Delta and B-2 Sigma(-) states
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Collision-partner dependence of energy transfer between the CH A(2)Delta and B-2 Sigma(-) states

机译：CH A（2）Delta与B-2 Sigma（-）状态之间能量转移的碰撞伙伴依赖性

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摘要

We have investigated experimentally the collision-induced electronic energy transfer between the CH A(2)Delta and B(2)Sigma(-) states with the series of partners He, Ar, H-2, N-2, CO, and CO2. Single rovibronic states of either of the near-degenerate levels A(2)Delta, nu = 1, or B(2)Sigma(-), nu = 0, were prepared by laser excitation. Collisional transfer processes were monitored by detecting dispersed, time-resolved fluorescence from the initial and product states. The microscopic rate constants for vibronically resolved transfer between the A(2)Delta and B(2)Sigma(-) states, vibrational relaxation within the A state, and total removal to unobserved final products were determined for each partner. In line with previous work, we find that only CO and H, are efficient at total removal of CH A(2)Delta and B(2)Sigma(-), most probably through chemical reaction. CO2 is notably effective at A(2)Delta state vibrational relaxation, possibly through resonant vibrational energy transfer. All the partners cause transfer between CH A(2)Delta and B(2)Sigma(-). An important new observation is that their efficiencies are well correlated with the strength of long-range attractive forces, as revealed through a positive correlation of the Parmenter-Seaver type. The vibronic branchina to A(2)Delta, nu = 0 and 1 from B(2)Sigma(-), nu = 0 is found to be significantly collision-partner-dependent and not well predicted by energy gap scaling laws. We do not find any enhanced effectiveness in B(2)Sigma(-) to A(2)Delta coupling for those partners which form strongly bound intermediates, suggesting that this specific electronic channel is controlled by different regions of the potential energy surfaces.
机译：我们已经实验研究了CH A（2）Delta和B（2）Sigma（-）状态之间的碰撞诱导电子能量转移，该过程与一系列伙伴He，Ar，H-2，N-2，CO和CO2 。通过激光激发准备了近简并水平A（2）Delta nu = 1或B（2）Sigma（-）nu = 0的单转子振动状态。通过从初始状态和产品状态检测分散的，时间分辨的荧光来监测碰撞转移过程。确定了每个伙伴的A（2）Delta和B（2）Sigma（-）状态之间的，通过电子方式分辨的转移，在A状态内的振动弛豫以及未观察到的最终产物的总去除的微观速率常数的微观速率常数。与以前的工作一致，我们发现只有CO和H才最有可能通过化学反应完全去除CH A（2）Delta和B（2）Sigma（-）。 CO2可能通过共振振动能量转移，对A（2）Delta态振动弛豫特别有效。所有伙伴导致CH A（2）Delta和B（2）Sigma（-）之间的转移。一个重要的新发现是，它们的效率与远程吸引力的强度密切相关，正如Parmenter-Seaver类型的正相关所揭示的那样。发现到B（2）Sigma（-），nu = 0到A（2）Delta，nu = 0和1的振动支是显着依赖碰撞伙伴的，并且不能通过能隙定标定律很好地预测。我们没有发现任何增强的效力在B（2）Sigma（-）到A（2）Delta耦合对那些形成牢固结合的中间体的伙伴，表明该特定电子通道受势能表面的不同区域控制。

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