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量子控制冷散射挑战理论。

Quantum Controlled Cold Scattering Challenges Theory.

作者信息

Perreault William E, Zhou Haowen, Mukherjee Nandini, Zare Richard N

机构信息

Department of Chemistry, Stanford University, Stanford, California94305, United States.

出版信息

J Phys Chem Lett. 2022 Dec 1;13(47):10912-10917. doi: 10.1021/acs.jpclett.2c03038. Epub 2022 Nov 17.

Abstract

Our previous rotationally inelastic cold scattering experiments between state prepared D ( = 2, = 2, = 0) and He disagreed with theory, raising serious concerns about either our understanding of the anisotropic potential or the accuracy of the measurement. To further interrogate interactions between molecular hydrogen and atomic helium, we study the Δ = 1and Δ = 2 rotational relaxation of HD ( = 2, = 2, = 0) by collision with He. The two rotational transitions probe different anisotropic components of the van der Waals potential. Our state resolved scattering study shows that these two transitions are mediated by two different shape resonances = 1 for Δ = 1 and = 2 for Δ = 2. The strong = 1 resonance dominates the Δ = 1 scattering, agreeing with theory. However, the dominance of the weaker = 2 resonance in the Δ = 2 transition, which matches our earlier D-He result, contradicts theoretical calculations. The continued contradiction, when we expect one-to-one correspondence between our stereodynamically controlled scattering experiment and theoretical calculations, makes us question the accuracy of the weaker anisotropic part of the H-He interaction potential.

摘要

我们之前对处于态制备的 D(J = 2,M = 2,K = 0)与 He 之间进行的转动非弹性冷散射实验与理论不符,这引发了人们对我们对各向异性势的理解或测量精度的严重担忧。为了进一步探究分子氢与原子氦之间的相互作用,我们研究了 HD(J = 2,M = 2,K = 0)与 He 碰撞时的 ΔJ = 1 和 ΔJ = 2 的转动弛豫。这两个转动跃迁探测了范德华势的不同各向异性分量。我们的态分辨散射研究表明,这两个跃迁由两个不同的形状共振介导,对于 ΔJ = 1 为 J = 1,对于 ΔJ = 2 为 J = 2。强的 J = 1 共振主导了 ΔJ = 1 散射,与理论相符。然而,较弱的 J = 2 共振在 ΔJ = 2 跃迁中的主导地位与理论计算相矛盾,这与我们早期 D-He 的结果一致。当我们期望在我们的立体动力学控制散射实验与理论计算之间存在一一对应关系时,持续存在的矛盾使我们质疑 H-He 相互作用势较弱各向异性部分的准确性。

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