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Metastable liquid-liquid phase transition in a single-component system with only one crystal phase and no density anomaly

机译:单组分系统中的亚稳液 - 液相变   只有一个晶相,没有密度异常

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摘要

We investigate the phase behavior of a single-component system in 3dimensions with spherically-symmetric, pairwise-additive, soft-coreinteractions with an attractive well at a long distance, a repulsive soft-coreshoulder at an intermediate distance, and a hard-core repulsion at a shortdistance, similar to potentials used to describe liquid systems such ascolloids, protein solutions, or liquid metals. We showed [Nature {\bf 409}, 692(2001)] that, even with no evidences of the density anomaly, the phase diagramhas two first-order fluid-fluid phase transitions, one ending in agas--low-density liquid (LDL) critical point, and the other in agas--high-density liquid (HDL) critical point, with a LDL-HDL phase transitionat low temperatures. Here we use integral equation calculations to explore the3-parameter space of the soft-core potential and we perform molecular dynamicssimulations in the interesting region of parameters. For the equilibrium phasediagram we analyze the structure of the crystal phase and find that, within theconsidered range of densities, the structure is independent of the density.Then, we analyze in detail the fluid metastable phases and, by explicitthermodynamic calculation in the supercooled phase, we show the absence of thedensity anomaly. We suggest that this absence is related to the presence ofonly one stable crystal structure.
机译:我们研究球状对称,成对加成,软核相互作用的3维单组分系统的相行为,该相互作用在长距离具有吸引力,在中间距离具有排斥性的软核肩部,并且具有硬核排斥性在短距离内,类似于描述液体系统(例如胶体,蛋白质溶液或液体金属)的电势。我们显示[Nature {\ bf 409},692(2001)],即使没有证据表明密度异常,该相图也有两个一阶流体相变,其中一个以气-低密度液体( LDL)临界点,另一个是气-高密度液体(HDL)临界点,在低温下具有LDL-HDL相变。在这里,我们使用积分方程计算来探究软核电势的三参数空间,并在有趣的参数范围内执行分子动力学模拟。对于平衡相图,我们分析了晶相的结构,发现在密度范围内,该结构与密度无关。然后,我们详细分析了流体亚稳相,并通过过冷相的显式热力学计算,我们显示没有密度异常。我们建议这种缺乏与仅一种稳定的晶体结构的存在有关。

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