快速升温步骤作为对Tool-Narayanaswamy形式主义的检验
Fast temperature up steps as a test of the Tool-Narayanaswamy formalism
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中文总结 AI 辅助
研究玻璃形成液体TEAC在快速升温步骤后的老化动力学，通过实验确定Tool-Narayanaswamy形式主义的参数，测试其预测能力，发现小幅度步骤预测效果好，大幅度步骤效果差，探讨了该形式主义有效性极限通用标准的可能性。
中文摘要 AI 辅助
我们研究了玻璃形成液体三乙基-2-乙酰柠檬酸酯（TEAC）在幅度为0.3至13.6K的快速升温步骤后的老化动力学。初始状态要么处于平衡态，要么通过先前的降温步骤实验在不同程度的非平衡态下制备。目标是检验Tool-Narayanaswamy（TN）形式主义的预测能力，该形式主义假设液体的非线性再平衡可与其对小扰动的线性响应相关联。我们确定了小到中等幅度（≤3.3K）步骤的TN参数，并利用低于玻璃化转变温度的降温步骤老化实验来约束平衡弛豫时间的确定。我们测试了TN预测，发现对于表征与平衡距离高达10K的虚构温度差异，一致性非常好。然而，对于更大的步骤，预测逐渐无法捕捉老化动力学。这可能表明再平衡机制不再与平衡动力学相关。最后，我们讨论了获得TN形式主义有效性极限通用标准的可能性，并与文献中的其他系统进行了比较。
英文摘要
We investigated the aging dynamics of a glass-forming liquid triethyl-2-acetylcitrate (TEAC), following fast temperature up steps with amplitudes ranging from 0.3 to 13.6 K. The initial states were either at equilibrium or prepared at increasing levels of out-of-equilibrium through a prior down step experiment. Our goal was to test the predictive power of the Tool-Narayanaswamy (TN) formalism which assumes that the non-linear re-equilibration of a liquid can be linked to its linear response to a small perturbation. We determined the TN parameters for steps with small to moderate amplitude ($\leq$ 3.3 K) and crucially took advantage of down step aging experiments below the glass transition temperature to constrain the determination of the equilibrium relaxation time. We tested the TN predictions and found very good agreement for differences in fictive temperature characterizing the distance from equilibrium as high as 10 K. For larger steps, however, the prediction progressively fails to capture the aging dynamics. This likely indicates that the re-equilibration mechanism is no longer related to the equilibrium dynamics. Finally, we discuss the possibility of obtaining a general criterion for the limit of validity of the TN formalism, which we compare to other systems from the literature.
