等温引入2nm结构不均匀性引起的分子液体弛豫模的退耦
On the decoupling of relaxation modes in a molecular liquid caused by isothermal introduction of 2nm structural inhomogeneities
摘要：
为了支持一个新的解释的起源普遍观察到的动态异质性在脆弱的液体，因为他们接近他们的玻璃化转变温度Tg，我们表明，引入~2 nm的结构不均匀性到一个均匀的玻璃形成导致解耦的扩散从粘度类似的邻三联苯OTP低于TA的冷却过程中所观察到的，其中Arrhenius行为丢失。此外，解耦效应随着温度降低（和粘度增加）而变得更强。液体是甲酚，并且~2nm的不均匀物是甲酚可溶的不对称衍生的基于四氢呋喃（POSS）的分子。退耦是Onsager在讨论随着温度降低的液-液相分离方法时预测的现象。在这种情况下，观察结果支持了隐藏在玻璃化转变之下的易碎液体中的多晶转变的概念。当球状蛋白溶解在稀水溶液或质子离子液体中时，可以预期类似的解耦。
英文摘要：
To support a new interpretation of the origin of the dynamic heterogeneity observed pervasively in fragile liquids as they approach their glass transition temperatures Tg, we demonstrate that the introduction of ~2 nm structural inhomogeneities into a homogeneous glassformer leads to a decoupling of diffusion from viscosity similar to that observed during the cooling of orthoterphenyl OTP below TA, where Arrhenius behavior is lost. Further, the decoupling effect grows stronger as temperature decreases (and viscosity increases). The liquid is cresol and the ~2nm inhomogeneities are cresol-soluble asymmetric derivatized tetrasiloxy-based (POSS) molecules. The decoupling is the phenomenon predicted by Onsager in discussing the approach to a liquid-liquid phase separation with decreasing temperature. In the present case the observations support the notion of a polyamorphic transition in fragile liquids that is hidden below the glass transition. A similar decoupling can be expected as a globular protein is dissolved in dilute aqueous solutions or in protic ionic liquids.
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