论文标题
用分层机学习电势了解高压氢
Understanding high pressure hydrogen with a hierarchical machine-learned potential
论文作者
论文摘要
氢相图具有许多异常特征,这些特征通常通过密度功能计算很好地重现。不幸的是,这些计算无法就这些特征发生的原因提供良好的物理见解。在本文中,我们将允许长和大模拟的分子氢的模型参数化。该模型显示了相图的出色繁殖,包括损坏的对称相位II,有效包装的III期以及熔体曲线中的最大值。它还可以很好地复制振动频率,包括振动频率$ν(P)$的最大值和负热膨胀。通过详细研究冗长的分子动力学,我们为观察到的特性提供了直观的解释。所有固体结构近似于六角形关闭,并通过分子方向打破对称性。在高压下,I期在分子方向之间显示出显着的短距离相关性。拉曼频率的营业额是由于相邻分子之间的耦合增加,而不是键的键。该液体比近距离包装的固体更密集,因为在2.3Å的分子分离下,受欢迎的相对方向从四极杆 - 能量最小化到定位 - 抑制 - 最小化。后者允许分子靠近,而不会靠近原子,但在封闭层的限制内无法实现这一目标。
The hydrogen phase diagram has a number of unusual features which are generally well reproduced by density functional calculations. Unfortunately, these calculations fail to provide good physical insights into why those features occur. In this paper, we parameterize a model potential for molecular hydrogen which permits long and large simulations. The model shows excellent reproduction of the phase diagram, including the broken-symmetry Phase II, an efficiently-packed phase III and the maximum in the melt curve. It also gives an excellent reproduction of the vibrational frequencies, including the maximum in the vibrational frequency $ν(P)$ and negative thermal expansion. By detailed study of lengthy molecular dynamics, we give intuitive explanations for observed and calculated properties. All solid structures approximate to hexagonal close packed, with symmetry broken by molecular orientation. At high pressure, Phase I shows significant short-ranged correlations between molecular orientations. The turnover in Raman frequency is due to increased coupling between neighboring molecules, rather than weakening of the bond. The liquid is denser than the close-packed solid because, at molecular separations below 2.3Å, the favoured relative orientation switches from quadrupole-energy-minimising to steric-repulsion-minimising. The latter allows molecules to get closer together, without atoms getting closer but this cannot be achieved within the constraints of a close-packed layer.