分子动力学模拟中的液态玻璃观测

Mohammed Alhissi, Andreas Zumbusch, Matthias Fuchs
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引用次数: 0

摘要

分子各向异性在液体的玻璃化转变过程中起着重要作用。最近,通过对椭圆形胶体悬浮液进行光学显微镜实验,发现了一种新型的块状玻璃态。"液态玻璃 "是向列液晶的无序类似物,其中的旋转运动受到阻碍,但粒子可以自由扩散。当排列整齐的粒子群相互交织时,全局向列有序被抑制。我们进行了布朗动力学模拟,以测试软椭圆形粒子密集系统的结构和动力学。正如在实验中看到的那样,根据模式耦合理论的预测,在我们模拟的时间尺度上,液态玻璃中的旋转运动被冻结,但平移运动却持续存在。对平移和旋转动态结构函数的分析证实了旋转和平移分别存在两个独立的玻璃跃迁。尽管平衡态应该是向列型的,但排列结构仍然很小,并且取向次序随着尺寸的增大而迅速减弱。长波长波动是各向同性-向列转变的残余。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Observation of liquid glass in molecular dynamics simulations
Molecular anisotropy plays an important role in the glass transition of a liquid. Recently, a novel bulk glass state has been discovered by optical microscopy experiments on suspensions of ellipsoidal colloids. “Liquid glass” is a disordered analog of a nematic liquid crystal, in which rotation motion is hindered but particles diffuse freely. Global nematic order is suppressed as clusters of aligned particles intertwine. We perform Brownian dynamics simulations to test the structure and dynamics of a dense system of soft ellipsoidal particles. As seen in the experiments and in accordance with predictions from the mode coupling theory, on the time scale of our simulations, rotation motion is frozen but translation motion persists in liquid glass. Analyses of the dynamic structure functions for translation and rotation corroborates the presence of two separate glass transitions for rotation and translation, respectively. Even though the equilibrium state should be nematic, aligned structures remain small and orientational order rapidly decays with increasing size. Long-wavelength fluctuations are remnants of the isotropic-nematic transition.
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