Demmel F, Jimenez-Ruiz M
ISIS Facility, Rutherford Appleton Laboratory, Didcot OX11 0QX, United Kingdom.
ILL, 71 Avenue des Martyrs, 38042 Grenoble Cedex 9, France.
Phys Rev E. 2022 Jul;106(1-1):014606. doi: 10.1103/PhysRevE.106.014606.
Liquid sulfur consists mainly of eight-membered rings and hence can be regarded as a model of a molecular liquid. A liquid, which is built from different molecular structures, will demonstrate a wide range in relaxation processes and excitation modes. Three inelastic neutron scattering experiments have been performed to study the collective dynamics of liquid sulfur over three decades in frequencies. A wide range of wave vectors was studied to reveal the response of density fluctuations over different lengthscales. A viscoelastic model with a two-times memory function was applied to the data. The analysis revealed a slow relaxation mode, an acoustic-type excitation, and a high-frequency mode, which resembles an optic-type excitation. The wave-vector dependence of the slow relaxation mode width exhibits the signs of a de Gennes narrowing around the wave vector where the structure factor has a shoulder. This slow relaxation process could be related to diffusive particle movements. The acoustic-type modes evidence a viscoelastic reaction with a 50% enhancement of the sound velocity. This enhancement of the sound velocity and the spectral line shape is qualitatively similar to spectra of molecular liquids. The two relaxation times of the memory function are separated by about two orders of magnitude and underpin the need for a wide frequency range investigation of this complex liquid. The high-frequency response can be interpreted as optic-type modes in the liquid.
液态硫主要由八元环组成,因此可被视为分子液体的一个模型。由不同分子结构构成的液体,在弛豫过程和激发模式方面会表现出很大的差异。已进行了三项非弹性中子散射实验,以研究液态硫在三个数量级频率范围内的集体动力学。研究了广泛的波矢范围,以揭示不同长度尺度下密度涨落的响应。将具有双时记忆函数的粘弹性模型应用于这些数据。分析揭示了一种慢弛豫模式、一种声学型激发以及一种类似于光学型激发的高频模式。慢弛豫模式宽度的波矢依赖性在结构因子有一个肩部的波矢附近呈现出德热纳窄化的迹象。这种慢弛豫过程可能与扩散性粒子运动有关。声学型模式表明存在一种粘弹性反应,声速提高了50%。声速的这种提高以及谱线形状在定性上与分子液体的光谱相似。记忆函数的两个弛豫时间相差约两个数量级,这表明需要对这种复杂液体进行宽频率范围的研究。高频响应可解释为液体中的光学型模式。