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聚合物微球中达到理想玻璃态:热力学与态密度振动分析

Reaching the Ideal Glass in Polymer Spheres: Thermodynamics and Vibrational Density of States.

作者信息

Monnier Xavier, Colmenero Juan, Wolf Marcel, Cangialosi Daniele

机构信息

Donostia International Physics Center, Paseo Manuel de Lardizabal 4, 20018 San Sebastián, Spain.

Departamento de Fisica de Materiales (UPV/EHU), Apartado 1072, 20080 San Sebastián, Spain.

出版信息

Phys Rev Lett. 2021 Mar 19;126(11):118004. doi: 10.1103/PhysRevLett.126.118004.

Abstract

The existence of an ideal glass and the resolution to the Kauzmann paradox is a long-standing open question in materials science. To address this problem, we exploit the ability of glasses with large interfacial area to access low energy states. We submit aggregates of spheres of a polymeric glass former to aging well below their glass transition temperature, T_{g}; and characterize their thermodynamic state by calorimetry, and the vibrational density of state (VDOS) by inelastic neutron scattering (INS). We show that, when aged at appropriate temperatures, glassy spheres attain a thermodynamic state corresponding to an ideal glass in time scales of about one day. In this state, the boson peak, underlying the deviation from the Debye level of the VDOS, is essentially suppressed. Our results are discussed in the framework of the link between the macroscopic thermodynamic state of glasses and their vibrational properties.

摘要

理想玻璃的存在以及考兹曼悖论的解决是材料科学中一个长期悬而未决的开放性问题。为了解决这个问题,我们利用具有大界面面积的玻璃进入低能态的能力。我们将一种聚合玻璃形成体的球体聚集体在远低于其玻璃化转变温度(T_{g})的条件下进行老化处理;通过量热法表征其热力学状态,并通过非弹性中子散射(INS)表征其振动态密度(VDOS)。我们表明,当在适当温度下老化时,玻璃态球体在大约一天的时间尺度内达到对应于理想玻璃的热力学状态。在这种状态下,作为VDOS偏离德拜能级基础的玻色子峰基本被抑制。我们在玻璃的宏观热力学状态与其振动特性之间联系的框架内讨论了我们的结果。

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