Sáez-Rábanos V, Verdasco J E, Herrero V J
Departamento de Sistemas y Recursos Naturales, E.T.S. de Ingeniería de Montes, Forestal y del Medio Natural, Universidad Politécnica de Madrid, 28040 Madrid, Spain.
Departamento de Química Física, Facultad de Química, Universidad Complutense de Madrid (Unidad Asociada CSIC), 28040 Madrid, Spain.
Phys Chem Chem Phys. 2019 Jul 10;21(27):15177-15186. doi: 10.1039/c9cp02718a.
Time-independent, fully converged, quantum dynamical calculations have been performed for the F + HD (v = 0, j = 0) and F + HD (v = 1, j = 0) reactions on an accurate potential energy surface down to collision energies of 0.01 meV. The two isotopic exit channels, HF + D and DF + H, have been investigated. The calculations reproduce satisfactorily the Feshbach resonance structures for collision energies between 10 and 40 meV, previously reported in the literature for the HF + D channel. Contrary to the results of a former literature work, vibrational excitation of HD is found to enhance reactivity in all cases down to the lowest collision energy investigated. Shape-type orbiting resonances are found for collision energies lower than 2 meV. The resonances appear as peaks in the reaction cross sections that are associated to specific values of the total angular momentum, J. In contrast with the Feshbach resonances at higher energies, the orbiting resonance structure, which is caused by the van der Waals well of the entrance channel, is identical for the HF + D and DF + H exit channels. The orbiting resonance peaks for F + HD (v = 0) are very small, but those for F + HD (v = 1) could be observed, in principle, with a combination of Raman pumping and merged beams methods.
已在精确的势能面上对F + HD(v = 0,j = 0)和F + HD(v = 1,j = 0)反应进行了与时间无关的、完全收敛的量子动力学计算,碰撞能量低至0.01 meV。对两个同位素出射通道HF + D和DF + H进行了研究。计算结果令人满意地再现了文献中先前报道的HF + D通道在10至40 meV碰撞能量之间的费什巴赫共振结构。与先前文献工作的结果相反,发现HD的振动激发在所有情况下都会增强反应性,直至所研究的最低碰撞能量。对于低于2 meV的碰撞能量,发现了形状型轨道共振。这些共振表现为反应截面中的峰值,与总角动量J的特定值相关。与较高能量下的费什巴赫共振不同,由入射通道的范德瓦尔斯阱引起的轨道共振结构对于HF + D和DF + H出射通道是相同的。F + HD(v = 0)的轨道共振峰非常小,但原则上,通过拉曼泵浦和合并束方法的组合可以观察到F + HD(v = 1)的轨道共振峰。