a priori path integral simulation on the dynamical properties and phenomena of low-temperature quantum molecular systems

低温量子分子系统动力学性质和现象的先验路径积分模拟

• 批准号: 14540472
• 负责人: KINUGAWA Kenichi
• 金额: $ 2.05万
• 依托单位: Nara Women's University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 2002
• 资助国家: 日本
• 起止时间: 2002 至 2003
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-14540472/
• 关键词: path integral; centroid molecular dynamics; liquid hydrogen; solid hydrogen; phonon; transport properties; structure factor; 構造因子; セントロイド分子動力学; 量子効果; フォノン分散; 動的構造因子

In the present series of studies, the static and dynamical properties of solid and liquid hydrogen have been non-empirically investigated by means of path integral centroid molecular dynamics (CMD) simulations.For solid para-hydrogen, we have obtained the phonon excitations with higher energies than those in previous experimental reports. Although the phonon dispersion in the high energy region in solid para-hydrogen has been definitely determined because of contradictory data reported from the experiments, our present study have thrown an insight into this outstanding controversy.The fundamental transport properties (self-diffusion coefficient, thermal conductivity, shear viscosity, and bulk viscosity) have been evaluated by using the CMD simulations. This work is the first attempt to numerically a priori estimate collective transport properties of any quantum liquids. In particular, the agreement of calculated self-diffusion coefficient and the shear viscosity with experimental values is excellent. On the other hand, the classical molecular dynamics simulations have yield the values much deviated from the experimental ones. This indicates that the essential features of the transport properties of liquid para-hydrogen comes from the quantum effect.The present series of studies are remarkable in that they have resolved the dynamical properties which cannot be revealed by any other computational techniques.

在本系列研究中，通过路径积分质心分子动力学（CMD）模拟对固体和液体氢的静态和动力学性质进行了非经验研究。对于固体para-Hydragen，我们获得了比以前的实验报告中具有更高能量的呼射子激发。尽管由于实验报告了相互矛盾的数据，因此确定了固体para-Hydragen的高能区域中的声子分散，但我们本研究对这一杰出的争议有了深入的了解。基本的运输属性（自传导系数，导热率，剪切粘度和散装粘度）已通过使用CMD进行了评估。这项工作是任何量子液体的先验估计集体运输特性的首次尝试。特别是，计算出的自扩散系数和实验值的剪切粘度的一致性非常好。另一方面，经典的分子动力学模拟产生的值与实验偏差很大。这表明液体para-hydrogen的运输特性的基本特征来自量子效应。目前的研究非常明显，因为它们已经解决了任何其他计算技术无法揭示的动力学特性。

项目成果

Hiroaki Saito, Hidemi Nagao, Kiyoshi Nishikawa, Kenichi Kinugawa: "Molecular collective dynamics in solid para-hydrogen and ortho-deuterium : the Parrinello-Rahman-type path integral centroid molecular dynamics approach"J.Chem.Phys. 119. 953 (2003)

Hiroaki Saito、Hidemi Nagao、Kiyoshi Nishikawa、Kenichi Kinukawa：“固体仲氢和邻氘中的分子集体动力学：Parrinello-Rahman 型路径积分质心分子动力学方法”J.Chem.Phys。

J.Dawidowski, F.J.Bermejo, M.L.Ristig, B.Fak, C.Cabrillo, R.Fernandez-Perea, K.Kinugawa, J.Campo: "Static structure factor of liquid parahydrogen"Phys.Rev.B. 69. 014207 (2004)

J.Dawidowski、F.J.Bermejo、M.L.Ristig、B.Fak、C.Cabrillo、R.Fernandez-Perea、K.Kinukawa、J.Campo：“液体仲氢的静态结构因子”Phys.Rev.B。

J.Dawidowski, F.J.Bermejo, Kinugawa: "Static structure factor of liquid parahydrogen"Physical Review B. 69. 014207-1-014207-7 (2004)

J.Dawidowski、F.J.Bermejo、鬼怒川：“液体仲氢的静态结构因子”物理评论 B. 69. 014207-1-014207-7 (2004)

Hiroaki Saito, Hidemi Nagao, Kiyoshi Nishikawa, Kenichi Kinugawa: "Molecular collective dynamics in solid para-hydrogen and ortho-deuterium : the Parrinello-Rahman-type path integral centroid molecular dynamics"The Journal of Chemical Physics. 119(2). 953

Hiroaki Saito、Hidemi Nagao、Kiyoshi Nishikawa、Kenichi Kinukawa：“固体仲氢和邻氘中的分子集体动力学：Parrinello-Rahman 型路径积分质心分子动力学”化学物理学杂志。

Yoshiteru Yonetani, Kenchi Kinugawa: "Transport properties of liquid para-hydrogen : the path integral centroid molecular dynamics approach"J.Chem.Phys.. 119. 9651 (2003)

Yoshiteru Yonetani、Kenchi Kinukawa：“液体仲氢的传输特性：路径积分质心分子动力学方法”J.Chem.Phys.. 119. 9651 (2003)