从体积测量洞察大尺寸玻璃形成体的性质
Insight into properties of sizable glass former from volumetric measurements
AI总结：
本研究针对大尺寸玻璃形成体玻璃化转变动力学的未解问题，结合PVT状态方程分析结构弛豫时间，发现热能与自由体积涨落对其分子重取向动力学几乎同等重要，修正了高压敏参数对应体积主导作用的认知。
摘要：
大尺寸玻璃形成体具有诸多独特性质与潜在应用，但关于其玻璃化转变动力学的诸多问题仍未得到解决。本研究结合压力-体积-温度（PVT）测量得到的状态方程，分析了随温度和压力变化的结构弛豫时间。尽管此前介电研究的证据表明过冷动力学对压缩具有显著敏感性，且与直觉相反，我们的结果为热能与自由体积涨落在控制大尺寸分子重取向动力学方面几乎同等重要提供了温和的证据。研究发现的标度指数为3.0，Ev/Ep比值为0.6，这对于弛豫动力学由两种效应共同决定且热涨落参与度略占优势的玻璃形成材料而言是典型的。研究表明，表征玻璃化转变动力学对压力变化敏感性的关键参数（即活化体积和dTg/dP）的高值，并非体积对玻璃化转变动力学有显著贡献的有效前提。
英文摘要：
Sizable glass formers feature numerous unique properties and potential applications, but many questions regarding their glass transition dynamics have not been resolved yet. Here we analyzed structural relaxation times measured as a function of temperature and pressure in combination with the equation of state obtained from pressure-volume-temperature (PVT) measurements. Despite evidence from previous dielectric studies indicating a remarkable sensitivity of supercooled dynamics to compression, and contrary to intuition, our results demonstrated the temperate proof for the almost equivalent importance of thermal energy and free volume fluctuations in controlling reorientation dynamics of sizable molecules. The found scaling exponent equals 3.0 and Ev/Ep ratio of 0.6 were typical for glass-forming materials with relaxation dynamics determined by both effects with a minor advantage of thermal fluctuations involvement. It shows that the high values of key parameters characterizing the sensitivity of the glass transition dynamics to pressure changes, i.e. activation volume and dTg/dP, are not a valid premise for a remarkable contribution of volume on glass transition dynamics.
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