Department of Physics and Physical Oceanography, Memorial University of Newfoundland, St. John's, NL, A1B 3X7, Canada.
Phys Rev Lett. 2009 Nov 27;103(22):225701. doi: 10.1103/PhysRevLett.103.225701. Epub 2009 Nov 23.
In simulations of supercooled, high-density liquid silica we study a range of temperature T in which we find both crystal nucleation as well as the characteristic dynamics of a glass forming liquid, including a breakdown of the Stokes-Einstein relation. We find that the liquid cannot be observed below a homogeneous nucleation limit (HNL) at which the liquid crystallizes faster than it can equilibrate. We show that the HNL would occur at lower T, and perhaps not at all, if the Stokes-Einstein relation were obeyed, and hence that glassy dynamics plays a central role in setting a crystallization limit on the liquid state in this case. We also explore the relation of the HNL to the Kauzmann temperature, and test for spinodal-like effects near the HNL.
在过冷、高密度液体硅的模拟中,我们研究了一系列温度 T,在这些温度下,我们发现了晶体成核以及玻璃形成液体的特征动力学,包括斯托克斯-爱因斯坦关系的破裂。我们发现,在均相成核极限 (HNL) 以下,液体不能被观察到,在这个极限下,液体的结晶速度比其达到平衡的速度快。我们表明,如果遵守斯托克斯-爱因斯坦关系,HNL 将在更低的温度下发生,或者根本不会发生,因此在这种情况下,玻璃态动力学在为液体状态设定结晶极限方面起着核心作用。我们还探讨了 HNL 与考夫曼温度的关系,并在 HNL 附近测试了类似旋节线的效应。