Tanaka H
Institute of Industrial Science, University of Tokyo, Meguro-ku, Tokyo 153-8505, Japan.
Phys Rev E Stat Phys Plasmas Fluids Relat Interdiscip Topics. 2000 Nov;62(5 Pt B):6968-76. doi: 10.1103/physreve.62.6968.
We present a general view of a liquid-liquid phase transition, based on a simple physical picture that there is "cooperative medium-range bond ordering" for any liquids. Contrary to the common belief, we argue that liquid is not homogeneous and in any liquid there exist locally favored structures, which are frustrated with normal-liquid structures. The cooperative excitation of locally favored structures leads to a gas-liquid-like critical point of bond ordering. This picture naturally leads to the conclusion that liquid-liquid transition is not specific to special materials, but can in principle exist in any liquids. Our model suggests a new possibility that (i) even an ordinary molecular liquid can have a hidden liquid-liquid phase transition and (ii) it may be the origin of a second amorphous phase (e.g., "glacial phase") and critical-like, large-scale fluctuations ("Fischer clusters") observed in supercooled molecular liquids.
我们基于一个简单的物理图像,即任何液体都存在“协同中程键序”,给出了液 - 液相转变的一般观点。与普遍看法相反,我们认为液体并非均匀的,在任何液体中都存在局部有利结构,这些结构与正常液体结构相互矛盾。局部有利结构的协同激发导致键序出现类似气 - 液的临界点。这一图像自然地得出结论:液 - 液相转变并非特定材料所特有,原则上可以存在于任何液体中。我们的模型提出了一种新的可能性,即(i)即使是普通分子液体也可能存在隐藏的液 - 液相转变,以及(ii)它可能是在过冷分子液体中观察到的第二非晶相(例如“冰状相”)和类似临界的大规模涨落(“费舍尔簇”)的起源。