Forrest J A, Dalnoki-Veress K
Department of Physics and Astronomy, University of Waterloo, Waterloo, Ontario, Canada, N2L 3G1.
Perimeter Institute for Theoretical Physics, 31 Caroline Street N., Waterloo, Ontario, Canada, N2L 2Y5.
ACS Macro Lett. 2014 Apr 15;3(4):310-314. doi: 10.1021/mz4006217. Epub 2014 Mar 17.
We present a simple model that links enhanced mobility at the free surface to the dilatometric glass transition temperature, in thin films. The model shows that what is typically measured as a dilatometric , characterized by the hallmark "kink" in the plot of film thickness versus temperature, only represents the dynamics of an infinitesimally thin layer of the sample. In other words, the measured dilatometric value in thin films is no longer a good reporter of the dynamics. Calculations based on the model are found to agree with a vast body of thin film measurements. While mathematically simple, the model contains all the necessary physics of a near surface layer with enhanced dynamics and a length scale over which the surface dynamics monotonically varies from surface enhanced to bulk-like. The model demonstrates that the typical dilatometric measurement of the glass transition is not necessarily a real glass transition.
我们提出了一个简单的模型,该模型将薄膜自由表面处增强的迁移率与膨胀计玻璃化转变温度联系起来。该模型表明,通常作为膨胀计测量的结果,其特征是薄膜厚度与温度关系图中的标志性“扭结”,仅代表样品中一个无限薄的层的动力学。换句话说,薄膜中测得的膨胀计值不再是动力学的良好指标。基于该模型的计算结果与大量薄膜测量结果相符。虽然该模型在数学上很简单,但它包含了近表面层所有必要的物理特性,即具有增强的动力学以及一个长度尺度,在该长度尺度上表面动力学从表面增强状态单调变化到类似体相的状态。该模型表明,玻璃化转变的典型膨胀计测量结果不一定是真正的玻璃化转变。