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Comment on 'An experimental critique on the existence of fragile-to-strong transition in glass-forming liquids'

机译:评论“玻璃形成液体脆弱过渡存在的实验批评”

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In a recent article, Zhu et al. suggest that a discrepancy exist between viscosity measurements performed by oscillation viscometry compared to other techniques such as capillary or parallel plate methods. They argue that oscillation viscometry data increasingly deviate with temperature leading to a systematic mismatch at high temperature. They conclude that this discrepancy discredit the existence of most fragile-to-strong transitions (FST) reported recently that are based on this type of measurement. Here we show that when all the data available are taken into account, this argument loses its coherency. Indeed, if FST were an artefact of instrumental error then all liquids measured using oscillation viscometry over the same temperature and viscosity range should exhibit an apparent FST. Instead, data available at high temperature for Se shows no FST but in fact show an excellent match with model prediction over the full temperature range, while data for GeSe3 measured over the same range show a severe kink revealing an FST which therefore cannot be assigned to a mismatch between measurement techniques. Furthermore we show that oscillation viscometry data can be independently corroborated using heat capacity data via the Adam Gibbs equation. Finally we show that large vapor pressure losses occur in Ge-Se glasses at high temperature and are likely responsible for the reported deviation in viscosity measurement. This is not the case of oscillation viscometry measurements that are performed in sealed ampoules. Overall these results confirm the validity of oscillation viscometry as well as the existence of fragile-to-strong transitions.
机译:在最近的一篇文章中,朱等人。建议与振荡粘度测量法相比,与其他技术(例如毛细管或平行板)相比,存在差异。他们认为,振荡粘度测定数据越来越偏离导致高温系统不匹配的温度。他们得出结论,这种差异诋毁最近报道的最脆弱的转变(FST)的存在,这是基于这种测量的。在这里,我们显示,当考虑所有可用数据时,此参数会失去其一致性。实际上,如果FST是乐器误差的人工制品,则使用在相同温度和粘度范围内使用振荡粘度测量的所有液体应表现出明显的FST。相反,对于SE的高温可用的数据显示了FST,但实际上表现出与全温范围内的模型预测的出色匹配,而在相同范围内测量的GESE3的数据显示出一个严重的扭结,因此不能分配FST测量技术之间的不匹配。此外,我们表明,振荡粘度测定数据可以通过ADAM Gibbs方程使用热容量数据独立证实。最后,我们表明在高温下在GE-SE眼镜中发生大的蒸气压损失,可能对报告的粘度测量偏差负责。这不是在密封安瓿中执行的振荡粘度测量的情况。总体而言,这些结果证实了振荡粘度率的有效性以及脆弱的转换的存在。

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