Wolynes Peter G
Departments of Physics and Chemistry and Biochemistry, Center for Theoretical Biological Physics, University of California at San Diego, La Jolla, CA 92093, USA.
Proc Natl Acad Sci U S A. 2009 Feb 3;106(5):1353-8. doi: 10.1073/pnas.0812418106. Epub 2009 Feb 2.
Complex spatiotemporal structures develop during the process of aging glasses after cooling and of rejuvenating glasses on heating. The key to understanding these structures is the interplay between the activated reconfiguration events that generate mobility and the transport of mobility. These effects are both accounted for by combining the random first-order transition theory of activated events with mode coupling theory in an inhomogeneous setting. The predicted modifications by mobility transport of the time course of the aging regime are modest. In contrast, the rejuvenation process is strongly affected through the propagation of fronts of enhanced mobility originating from the initial reconfiguration events. The structures in a rejuvenating glass resemble flames. An analysis along the lines of combustion theory provides an estimate of the front propagation speed. Heterogeneous rejuvenation naturally should occur for glasses with free surfaces. The analogy with combustion also provides a way of looking at the uptake of diluents by glasses described by case II and super case II diffusion.
复杂的时空结构在冷却后的老化玻璃过程以及加热时玻璃的年轻化过程中形成。理解这些结构的关键在于产生迁移率的活化重排事件与迁移率传输之间的相互作用。通过在非均匀环境中将活化事件的随机一级转变理论与模式耦合理论相结合,可以解释这些效应。迁移率传输对老化阶段时间进程的预测修正较小。相比之下,年轻化过程会受到源自初始重排事件的迁移率增强前沿传播的强烈影响。年轻化玻璃中的结构类似于火焰。沿着燃烧理论进行分析可以估算前沿传播速度。对于具有自由表面的玻璃,自然会发生非均匀年轻化。与燃烧的类比也提供了一种看待由情况II和超情况II扩散描述的玻璃对稀释剂吸收的方法。