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Induced cooperative motions in a medium driven at the nanoscale: Searching for an optimum excitation period

机译:在纳米尺度驱动的介质中诱导协同运动:寻找最佳激发周期

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摘要

Recent results have shown the appearance of induced cooperative motions called dynamic heterogeneity during the isomerization of diluted azobenzene molecules in a host glass-former. In this paper, we raise the issue of the coupling between these “artificial” heterogeneities and the isomerization period. How do these induced heterogeneities differ in the saturation regime and in the linear response regime? Is there a maximum of the heterogeneous motion versus the isomerization rate, and why? Is the heterogeneity evolution with the isomerization rate connected with the diffusion or relaxation time evolution? We use out-of-equilibrium molecular dynamics simulations to answer these questions. We find that the heterogeneity increases in the linear response regime for large isomerization periods and small perturbations. In contrast, the heterogeneity decreases in the saturation regime, i.e., when the isomerization half-period (τp /2) is smaller than the relaxation time of the material (τα). This result enables a test of the effect of cooperative motions on the dynamics using the chromophores as Maxwell demons that destroy or stimulate the cooperative motions. Because the heterogeneities increase in the linear regime and then decrease in the saturation regime, we find a maximum for τp /2 ≈ τα . The induced excitation concentration follows a power-law evolution versus the isomerization rate and then saturates. As a consequence, the α relaxation time is related to the excitation concentration with a power law, a result in qualitative agreement with recent findings in constrained models. This result supports a common origin for the heterogeneities with constrained models and a similar relation to the excitation concentration.
机译:最近的结果表明在宿主玻璃前体中稀释的偶氮苯分子异构化过程中出现了诱导的称为动态异质性的协同运动。在本文中,我们提出了这些“人工”异质性与异构化期之间的耦合问题。这些诱导的异质性在饱和状态和线性响应状态如何不同?异构运动相对于异构化速率是否存在最大值,为什么?具有异构化速率的异质性演化是否与扩散或弛豫时间演化相关?我们使用非平衡分子动力学模拟来回答这些问题。我们发现,对于较大的异构化周期和较小的扰动,线性响应方案中的异质性增加。相反,在饱和状态下,即当异构化半周期(τp/ 2)小于材料的弛豫时间(τα)时,异质性降低。该结果使得能够使用发色团作为破坏或刺激协同运动的麦克斯韦恶魔来测试协同运动对动力学的影响。因为异质性在线性状态下增加,然后在饱和状态下减少,所以我们找到了τp/ 2≈τα的最大值。诱导的激发浓度遵循幂律演化对异构化速率的关系,然后饱和。结果,α弛豫时间与幂定律相关的激发浓度有关,结果与约束模型中的最新发现在质量上吻合。该结果支持具有受约束模型的异质性的共同起源,并且与激发浓度具有相似的关系。

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  • 作者

    V. Teboul; J.B. Accary;

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  • 年度 2014
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  • 原文格式 PDF
  • 正文语种 eng
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