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Inelastic neutron scattering investigations of the quantum molecular dynamics of a H_2 molecule entrapped inside a fullerene cage

机译:富勒烯笼内截获的H_2分子的量子分子动力学的非弹性中子散射研究

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摘要

The quantum dynamics of dihydrogen molecules entrapped inside fullerene cages has been investigated using inelastic neutron scattering (INS). For the endofullerene H_2@C_(60) the low-lying energy levels of the manifold of coupled translational and rotational states have been accurately determined by studying INS spectra recorded in the temperature range 1.5≤T≤ 240 K. The majority of transitions observed in the INS spectra interconvert the nuclear spin isomers orthohydrogen and parahydrogen. The cage potential has icosahedral symmetry and splittings observed in the INS spectra reveal the coupling of translational and rotational angular momentum of the H_2 molecules. The effects of nuclear spin symmetry, isotope mass effects, and cage anisotropy have been further investigated by studying HD@C_(60) and H_2 inside an open cage endofullerene. The momentum transfer κ arising from the neutron scattering event has also been investigated. The κ-dependence spectra reflect the physical dimensions of the dihydrogen molecule and its confinement in its cage. We show how this may be used as a tool for assigning the INS transitions.
机译:使用非弹性中子散射(INS)研究了富勒烯笼中截留的二氢分子的量子动力学。对于内富勒烯H_2 @ C_(60),通过研究在1.5≤T≤240K的温度范围内记录的INS光谱,已精确确定了耦合的平移和旋转状态的歧管的低能级。 INS光谱将核自旋异构体原氢和副氢相互转化。笼势具有二十面体对称性,在INS光谱中观察到的分裂揭示了H_2分子的平移和旋转角动量的耦合。通过研究开放笼式富勒烯内的HD @ C_(60)和H_2,进一步研究了核自旋对称性,同位素质量效应和笼形各向异性的影响。还研究了中子散射事件引起的动量传递κ。 κ依赖性光谱反映了二氢分子的物理尺寸及其在笼中的限制。我们展示了如何将其用作分配INS过渡的工具。

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  • 来源
    《Physical review》 |2012年第20期|p.205440.1-205440.12|共12页
  • 作者单位

    School of Physics & Astronomy, University of Nottingham, Nottingham, NG7 2RD, United Kingdom;

    School of Physics & Astronomy, University of Nottingham, Nottingham, NG7 2RD, United Kingdom;

    lnstitut Laue-Langevin, BP 156, 38042 Grenoble, France;

    lnstitut Laue-Langevin, BP 156, 38042 Grenoble, France;

    lnstitut Laue-Langevin, BP 156, 38042 Grenoble, France;

    School of Chemistry, University of Southampton, Southampton, SO17 1BJ, United Kingdom;

    School of Chemistry, University of Southampton, Southampton, SO17 1BJ, United Kingdom;

    School of Chemistry, University of Southampton, Southampton, SO17 1BJ, United Kingdom;

    Institute for Chemical Research, Kyoto University, Kyoto 611-0011, Japan;

    Institute for Chemical Research, Kyoto University, Kyoto 611-0011, Japan;

    Department of Chemistry, Columbia University, New York, New York 10027, USA;

    Department of Chemistry, Columbia University, New York, New York 10027, USA;

    Department of Chemistry, Columbia University, New York, New York 10027, USA;

    Department of Chemistry, Columbia University, New York, New York 10027, USA;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    rotational analysis;

    机译:旋转分析;

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