论文标题
n $^+ $（$^3p_ {j_a} $）中的自旋轨道过渡
Spin-orbit transitions in the N$^+$($^3P_{J_A}$) + H$_2$ $\rightarrow$ NH$^+$($X^2Π$, $^4Σ^-$)+ H($^2S$) reaction, using adiabatic and mixed quantum-adiabatic statistical approaches
论文作者
论文摘要
标题反应的横截面和速率常数是针对N $^+$（$^3p_ {J_A} $）的所有自旋轨道状态，使用两种统计方法，一种纯绝热，另一个用于入口通道和产品通道的绝热处理量的量子捕获。这是通过使用对称性的基准集组合反应物通道中的电子（自旋和轨道）和核角动量的组合来制作的。为此，针对反应物和产品分别执行了准确的{\ it i ab intib}计算。在反应物通道中，已经糖尿病了三个最低的电子状态（无自旋轨道耦合），并且已经通过将n $^+$原子中的自旋轨道相互作用定位的模型引入了自旋轨道耦合，与{\ IT IT IT IT IT IT的计算}计算相比，在N $^+$原子中的旋转耦合。对于产品，已通过{\ it i ab intib}计算确定了11个纯绝热的自旋轨道状态。这样获得的反应速率常数与几个Ortho-H $ _2 $分数的可用实验数据非常吻合，假设自旋轨道状态的热初始分布。获得选定的自旋轨道$ J_A $状态的速率常数，以适当地验证自旋轨道效应以获得实验速率常数。
The cross section and rate constants for the title reaction are calculated for all the spin-orbit states of N$^+$($^3P_{J_A}$) using two statistical approaches, one purely adiabatic and the other one mixing quantum capture for the entrance channel and adiabatic treatment for the products channel. This is made by using a symmetry adapted basis set combining electronic (spin and orbital) and nuclear angular momenta in the reactants channel. To this aim, accurate {\it ab initio} calculations are performed separately for reactants and products. In the reactants channel, the three lowest electronic states (without spin-orbit couplings) have been diabatized, and the spin-orbit couplings have been introduced through a model localizing the spin-orbit interactions in the N$^+$ atom, which yields accurate results as compared to {\it ab initio} calculations including spin-orbit couplings. For the products, eleven purely adiabatic spin-orbit states have been determined with {\it ab initio} calculations. The reactive rate constants thus obtained are in very good agreement with the available experimental data for several ortho-H$_2$ fractions, assuming a thermal initial distribution of spin-orbit states. The rate constants for selected spin-orbit $J_A$ states are obtained, to provide a proper validation of the spin-orbit effects to obtain the experimental rate constants.
