高能碰撞中$\text{N}_2(\text{X}^1Σ_g^+)$ + $\text{O}({}^3\text{P})$和$\text{NO}(\text{X}^2Π)$ + $\text{N}({}^4\text{S})$体系的旋振特性QCT和主方程研究
Rovibrational-Specific QCT and Master Equation Study on $\text{N}_2(\text{X}^1Σ_g^+)$+$\text{O}({}^3\text{P})$ and $\text{NO}(\text{X}^2Π)$+$\text{N}({}^4\text{S})$ Systems in High-Energy Collisions
摘要：
本文采用准经典轨道（QCT）和主方程分析方法，对$\text{N}_2(\text{X}^1Σ_g^+)$ + $\text{O}({}^3\text{P})$和$\text{NO}(\text{X}^2Π)$ + $\text{N}({}^4\text{S})$体系的能量转移和离解机理进行了详细的研究.通过QCT获得的完整的状态-状态动力学数据集，允许在微观和宏观尺度上深入研究导致$\text{NO}$分子形成的Zel'dovich机制。主方程分析表明，在交换过程中，$\text{N}_2$和$\text{NO}$的低振动态对$\text{NO}$的形成和相应的$\text{N}_2$的消光具有主导作用.对于所考虑的温度范围内，它被发现，而近50%的解离过程中发生的$\text{N}_2$和$\text{NO}$的分子准稳态（QSS）制度，Zel'dovich反应的量为零。使用QSS近似来模拟Zel'dovich机制导致在高温范围内对$\text{NO}$生产的高估超过4倍。这一著名的近似的崩溃有深刻的后果的方法，严重依赖于QSS假设的有效性在高超音速应用。振转态布居动力学的研究揭示了不同化学体系之间的能量转移和解离过程的实质相似性，为在不显著损失准确性的情况下对其他化学体系使用降阶策略提供了有希望的物理基础。
英文摘要：
This work presents a detailed investigation of the energy transfer and dissociation mechanisms in $\text{N}_2(\text{X}^1Σ_g^+)$+$\text{O}({}^3\text{P})$ and $\text{NO}(\text{X}^2Π)$+$\text{N}({}^4\text{S})$ systems using rovibrational-specific quasi-classical trajectory (QCT) and master equation analyses. The complete set of state-to-state kinetic data, obtained via QCT, allows for an in-depth investigation of the Zel'dovich mechanism leading to the formation of $\text{NO}$ molecules at microscopic and macroscopic scales. The master equation analysis demonstrates that the low-lying vibrational states of $\text{N}_2$ and $\text{NO}$ have dominant contributions to the $\text{NO}$ formation and the corresponding extinction of $\text{N}_2$ through the exchange process. For the considered temperature range, it is found that while nearly 50% of the dissociation processes for $\text{N}_2$ and $\text{NO}$ occurs in the molecular quasi-steady-state (QSS) regime, the amount of the Zel'dovich reaction is zero. Using the QSS approximation to model the Zel'dovich mechanism leads to an overestimation of $\text{NO}$ production by more than a factor of 4 in the high-temperature range. The breakdown of this well-known approximation has profound consequences for the approaches that heavily rely on the validity of QSS assumption in hypersonic applications. The investigation of the rovibrational state population dynamics reveals substantial similarity among different chemical systems for the energy transfer and the dissociation processes, providing promising physical foundations for the use of reduced-order strategies to other chemical systems without significant loss of accuracy.
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