Crystal growth kinetics exhibit a fragility-dependent decoupling from viscosity.
In this paper we establish the temperature dependence of the kinetic coefficient associated with crystal growth into the supercooled liquid for a wide range of organic and inorganic materials. We show that the kinetic coefficient for crystal growth scales with the shear viscosity eta as eta(-xi) and that the exponent depends systematically on the fragility of the liquid. The greater the fragility (i.e., deviation away from an Arrhenius temperature dependence for eta), the larger the difference 1-xi. We argue that this breakdown in scaling between the crystal growth kinetics and the viscosity is a manifestation of heterogeneous dynamics in supercooled liquids. In addition, we show that the absolute growth rate at intermediate viscosities is correlated with the entropy difference between the liquid and the crystal.
Ediger
M D
MD
Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, USA.
Harrowell
Peter
P
Yu
Lian
L
D002627:Chemistry, Physical / Q000379:methods*; D003460:Crystallization; D019277:Entropy; D007477:Ions; D007700:Kinetics; D008094:Lithium; D008956:Models, Chemical; D015233:Models, Statistical; D013314:Stress, Mechanical; D013696:Temperature; D013816:Thermodynamics; D014783:Viscosity
D007477:Ions; D008094:Lithium