Bergeat A, Morales S B, Naulin C, Wiesenfeld L, Faure A
Université de Bordeaux, CNRS, Bordeaux INP, ISM, UMR5255, F-33405 Talence, France.
Université Paris-Saclay, CNRS, Laboratoire Aimé Cotton, F-91405 Orsay, France.
Phys Rev Lett. 2020 Oct 2;125(14):143402. doi: 10.1103/PhysRevLett.125.143402.
Molecular scattering at collisional energies of the order of 10-100 cm^{-1} (corresponding to kinetic temperatures in the 15-150 K range) provides insight into the details of the scattering process and, in particular, of the various resonances that appear in inelastic cross sections. In this Letter, we present a detailed experimental and theoretical study of the rotationally inelastic scattering of ground-state ortho-D_{2}O by ground-state para-H_{2} in the threshold region of the D_{2}O(0_{00}→2_{02}) transition at 35.9 cm^{-1}. The measurements were performed with a molecular crossed beam apparatus with variable collision angle, thence with variable collisional energy. Calculations were carried out with the coupled-channel method combined with a dedicated high-level D_{2}O-H_{2} intermolecular potential. Our theoretical cross section 0_{00}→2_{02} is found to display several resonance peaks in perfect agreement with the experimental work, in their absolute positions and relative intensities. We show that those peaks are mostly due to shape resonances, characterized here for the first time for a polyatomic molecule colliding with a diatom.
在碰撞能量约为10 - 100 cm⁻¹(对应15 - 150 K范围内的动力学温度)下的分子散射,能深入了解散射过程的细节,特别是非弹性截面中出现的各种共振。在本信函中,我们对基态仲氢(para - H₂)与基态邻重水(ortho - D₂O)在35.9 cm⁻¹的D₂O(0₀₀→2₀₂)跃迁阈值区域的转动非弹性散射进行了详细的实验和理论研究。测量使用了具有可变碰撞角(因而具有可变碰撞能量)的分子交叉束装置进行。计算采用耦合通道方法并结合专门的高精度D₂O - H₂分子间势进行。我们发现理论截面0₀₀→2₀₂在绝对位置和相对强度上与实验结果完美吻合,显示出几个共振峰。我们表明,这些峰主要归因于形状共振,这是首次针对与双原子分子碰撞的多原子分子进行此类表征。