Rehwald Christian, Gnan Nicoletta, Heuer Andreas, Schrøder Thomas, Dyre Jeppe C, Diezemann Gregor
Institut für Physikalische Chemie, Universität Münster, Federal Republic of Germany.
Phys Rev E Stat Nonlin Soft Matter Phys. 2010 Aug;82(2 Pt 1):021503. doi: 10.1103/PhysRevE.82.021503. Epub 2010 Aug 10.
We present molecular dynamics simulations of the binary Kob-Andersen Lennard-Jones model, a model glass former, and consider the distributions of inherent energies and metabasins during aging. In addition to the typical protocol of performing a temperature jump from a high temperature to a low destination temperature, we consider the temporal evolution of the energy distributions after an "up-jump," i.e., from a low to a high temperature. In this case, for times on the order of the relaxation time the distribution of metabasin energies exhibits a transient two-peak structure for a small system (65 particles). For a large system (1000 particles) no such two-peak structure appears because it is averaged out. The simulations show, however, that a clear signal of an intermediate two-peak structure survives in the thermodynamic limit, namely that the inherent energy distribution width goes through a maximum at intermediate times for temperature up jumps; no such maximum is found for temperature down jumps. These findings are qualitatively rationalized in terms of a simple trap model with a Gaussian distribution of energies, assuming that the liquid may be divided into non-interacting regions each of which is described by a trap model.
我们展示了二元Kob-Andersen Lennard-Jones模型(一种典型的玻璃形成模型)的分子动力学模拟,并考虑了老化过程中固有能量和亚稳态盆地的分布。除了从高温到低温目标温度进行温度跳跃的典型方案外,我们还考虑了“向上跳跃”(即从低温到高温)后能量分布的时间演化。在这种情况下,对于小系统(65个粒子),在弛豫时间量级的时间内,亚稳态盆地能量分布呈现出瞬态双峰结构。对于大系统(1000个粒子),由于这种结构被平均掉,所以没有出现这样的双峰结构。然而,模拟表明,在热力学极限下,中间双峰结构的清晰信号仍然存在,即对于温度向上跳跃,固有能量分布宽度在中间时间达到最大值;对于温度向下跳跃,则没有发现这样的最大值。这些发现通过一个具有高斯能量分布的简单陷阱模型在定性上得到了合理的解释,假设液体可以被划分为非相互作用区域,每个区域都由一个陷阱模型描述。