The Endofullerene HF@C60: Inelastic Neutron Scattering Spectra from Quantum Simulations and Experiment, Validity of the Selection Rule, and Symmetry Breaking.
The Endofullerene HF@C60: Inelastic Neutron Scattering Spectra from Quantum Simulations and Experiment, Validity of the Selection Rule, and Symmetry Breaking.
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Endofullerene HF@C60：来自量子模拟和实验的非弹性中子散射光谱、选择规则的有效性和对称性破缺。
DOI：
10.1021/acs.jpclett.9b02005
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Xu M
中科院分区：
文献类型：
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作者：
Xu M
报道了对两个入射中子波长的Hf@C60的低温非弹性中子散射(INS)谱的精确量子模拟。它们的区别在于在处理中严格包含了对称破缺效应，并且使用HF作为客体计算光谱，而不是像过去的工作那样使用H2或HD计算光谱。结果表明，尽管HF具有很大的质量不对称性和平移-旋转本征态的强烈混合特性，但开创先例的INS选择规则也适用于HF@C60，该规则最初是针对近球形纳米空间中的H2和HD推导的。这为之前的理论预测提供了重要的支持，即InS选择规则适用于近球形纳米约束中的任何双原子分子。选择规则在对称破缺的情况下仍然有效，但以一种有趣的方式进行了轻微的修改。并与最近发表的HF@C60的实验INS谱进行了比较。协议非常好，除了我们的计算建议重新分配的一个高峰。这种重新分配与本工作中测量的INS光谱是一致的，它覆盖了更大的能量范围。
Accurate quantum simulations of the low-temperature inelastic neutron scattering (INS) spectra of HF@C60are reported for two incident neutron wavelengths. They are distinguished by the rigorous inclusion of symmetry-breaking effects in the treatment and having the spectra computed with HF as the guest, rather than H2or HD, as in the past work. The results demonstrate that the precedent-setting INS selection rule, originally derived for H2and HD in near-spherical nanocavities, applies also to HF@C60, despite the large mass asymmetry of HF and the strongly mixed character of its translation–rotation eigenstates. This lends crucial support to the theoretical prediction made earlier that the INS selection rule is valid for any diatomic molecule in near-spherical nanoconfinement. The selection rule remains valid in the presence of symmetry breaking but is modified slightly in an interesting way. Comparison is made with the recently published experimental INS spectrum of HF@C60. The agreement is very good, apart from one peak for which our calculations suggest a reassignment. This reassignment is consistent with the measured INS spectrum presented in this work, which covers an extended energy range.