论文标题
精确复制基于内核的势能表面，用于n $ _2 $ o的三重态基态和n+n+no $ \ leftrightArrow $ o+n $ _2 $和n $ _2 $ _2 $+o $ $ $ $ 2N+o反应
Accurate Reproducing Kernel-Based Potential Energy Surfaces for the Triplet Ground States of N$_2$O and Dynamics for the N+NO$\leftrightarrow$O+N$_2$ and N$_2$+O$\rightarrow$2N+O Reactions
论文作者
论文摘要
已经确定了针对$^3 $ a $'$和$^3 $'$'$'$ _2 $ o的$^3 $ a $'$的准确势能表面（PESS）。超过20000 MRCI+Q/AUG-CC-PVTZ能量使用繁殖的内核Hilbert Space（RKHS）插值方案表示。 RKHS伙伴以高精度成功地描述了所有反应物通道。分析佩斯的特征是计算最小值和过渡状态。然后使用准经典动力学模拟来确定N+NO和O+N $ _2 $碰撞的热和振动放松率。从模拟和可用实验获得的结果之间的一致性对两种类型的观察物都有利，这提供了佩斯准确性的测试。 PESS可用于计算与高血压再入相关的更详细的状态对状态的可观察结果。
Accurate potential energy surfaces (PESs) have been determined for the $^3$A$'$ and $^3$A$''$ states of N$_2$O using electronic structure calculations at the multireference configuration interaction level with Davidson correction (MRCI+Q) and the augmented Dunning-type correlation consistent polarize triple zeta (aug-cc-pVTZ) basis set. More than 20000 MRCI+Q/aug-cc-pVTZ energies are represented using a reproducing kernel Hilbert space (RKHS) interpolation scheme. The RKHS PESs successfully describe all reactant channels with high accuracy. The analytical PESs are characterized by computing the minima and transition states on it. Quasiclassical dynamics simulations are then used to determine thermal and vibrational relaxation rates for the N+NO and O+N$_2$ collisions. The agreement between results obtained from the simulations and from available experiments is favourable for both types of observables, which provides a test for the accuracy of the PESs. The PESs can be used to calculate more detailed state-to-state observables relevant for applications to hypersonic reentry.
