Glass Dynamics Deep in the Energy Landscape
Glass Dynamics Deep in the Energy Landscape
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DOI：
10.1021/acs.jpcb.1c01739
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发表时间：
2021-08-06
影响因子：
3.3
通讯作者：
Wolynes, Peter G.
中科院分区：
文献类型：
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作者：
Ediger, Mark D.;Gruebele, Martin;Wolynes, Peter G.
当液体冷却时，能量景观的向下进展会在玻璃化转变温度 T-g 附近停止。原则上，可以通过等待进一步平衡来达到较低的能量状态，但玻璃的粗糙能量景观很快就会导致低于 T-g 的地质缓慢时间尺度上的动力学。在过去的十年中，通过多种技术对能源领域进行更深入的探索取得了进展。通过观察体积和表面扩散，使用促进平衡的分层沉积，以低于 T-g 的更快动力学对玻璃表面进行成像，以及光学激发玻璃，实验已经进入了过去难以获得的超稳定、低能量玻璃的状态。与此同时，基于随机一阶跃迁 (RFOT) 的模拟和能量景观理论都解决了包括表面、光学激发和界面动力学在内的系统。在这里，我们回顾了最近的一些实验工作，以及能量景观理论如何通过在构型熵、能量景观障碍和由此产生的动力学之间建立直接联系来阐明远低于玻璃化转变温度的玻璃态动力学。
When a liquid is cooled, progress down the energy landscape is arrested near the glass transition temperature T-g. In principle, lower energy states can be accessed by waiting for further equilibration, but the rough energy landscape of glasses quickly leads to kinetics on geologically slow time scales below T-g. Over the past decade, progress has been made probing deeper into the energy landscape via several techniques. By looking at bulk and surface diffusion, using layered deposition that promotes equilibration, imaging glass surfaces with faster dynamics below T-g, and optically exciting glasses, experiments have moved into a regime of ultrastable, low energy glasses that was difficult to access in the past. At the same time, both simulations and energy landscape theory based on a random first order transition (RFOT) have tackled systems that include surfaces, optical excitation, and interfacial dynamics. Here we review some of the recent experimental work, and how energy landscape theory illuminates glassy dynamics well below the glass transition temperature by making direct connections between configurational entropy, energy landscape barriers, and the resulting dynamics.