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Separation and conversion dynamics of nuclear-spin isomers of gaseous methanol

机译:气态甲醇核自旋异构体的分离与转化动力学

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All symmetrical molecules with non-zero nuclear spin exist in nature as nuclear-spin isomers (NSIs). However, owing to the lack of experimental information, knowledge is rare about interconversions of NSIs of gaseous molecules with torsional symmetry. Here we report our separation and conversion observations on NSI-torsion-specific transition systems of gaseous methanol from a light-induced drift experiment involving partially spatial separation of the ortho and para isomers. We find that vibrationally excited molecules of the methanol spin isomer have a smaller collision cross-section than their ground-state counterparts. Interconversion of the enriched ortho isomer with the para isomer, which is generally considered improbable, has been quantitatively studied by sensitive detections of the spectral intensities. Rather counterintuitively, this reveals that the interconversion is inhibited with increasing pressure. Our results suggest that the spin conversion mechanism in methanol is via a quantum relaxation process with the quantum Zeno effect induced by molecular collisions.
机译:自然界中具有非零核自旋的所有对称分子都以核自旋异构体(NSI)的形式存在。然而,由于缺乏实验信息,关于具有扭转对称性的气态分子的NSI相互转换的知识很少。在这里,我们从光诱导的漂移实验(涉及对位异构体和对位异构体的部分空间分离)报告了有关气态甲醇NSI扭转特定的过渡系统的分离和转化观察结果。我们发现,甲醇自旋异构体的振动激发分子比基态对应物具有更小的碰撞截面。富集的邻位异构体与对位异构体的相互转化(通常被认为是不可能的),已经通过光谱强度的灵敏检测进行了定量研究。相反,这反而表明,随着压力的增加,相互转化受到抑制。我们的结果表明,甲醇中的自旋转化机制是通过量子弛豫过程进行的,其中量子碰撞作用是由分子碰撞引起的。

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