论文标题

热膨胀和玻璃过渡

Thermal expansion and the glass transition

论文作者

Lunkenheimer, P., Loidl, A., Riechers, B., Zaccone, A., Samwer, K.

论文摘要

从Lindemann的标准来看,融化是充分理解的,基本上指出,当其原子的热振动变得如此剧烈以至于它们摆脱了结合力时,结晶材料融化了。但是,另一种常见的固体类型:玻璃,固体交叉的性质是高度争议的? Lindemann标准意味着晶体的热膨胀系数与它们的熔化温度成反比。在这里,我们发现,意外的是,玻璃的alpha降低了玻璃过渡温度TG的降低,标记了该材料类别中液体固定的交叉。然而,通过脆性m(粒子协作度的度量)缩放α,恢复了比例,即α/m〜1/tg。显然,要使玻璃成为液体,简单地克服颗粒间结合能就不足以成为液体。取而代之的是,必须投入更多的能量来打破典型的合作粒子网络,该网络被认为是玻璃材料的标志性特征。出乎意料的是,液相的α揭示了相似的异常行为,并以〜3的恒定因素的普遍增强。发现的普遍性允许从热膨胀中估算玻璃转换温度,反之亦然。

Melting is well understood in terms of the Lindemann criterion, essentially stating that crystalline materials melt when the thermal vibrations of their atoms become such vigorous that they shake themselves free of the binding forces. However, how about another common type of solids: glasses, where the nature of the solid-liquid crossover is highly controversial? The Lindemann criterion implies that the thermal expansion coefficients alpha of crystals are inversely proportional to their melting temperatures. Here we find that, unexpectedly, alpha of glasses decreases much stronger with increasing glass-transition temperature Tg marking the liquid-solid crossover in this material class. However, scaling alpha by the fragility m, a measure of particle cooperativity, restores the proportionality, i.e., alpha/m ~ 1/Tg. Obviously, for a glass to become liquid, it is not sufficient to simply overcome the interparticle binding energies. Instead, more energy has to be invested to break up the typical cooperative particle network which is considered a hallmark feature of glassy materials. Surprisingly, alpha of the liquid phase reveals similar anomalous behaviour and is universally enhanced by a constant factor of ~3. The found universalities allow estimating glass-transition temperatures from thermal expansion and vice versa.

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