Schirmacher Walter, Bryk Taras, Ruocco Giancarlo
Institut für Physik, Universität Mainz, D-55099 Mainz, Germany.
Center for Life Nano Science @Sapienza, Istituto Italiano di Tecnologia, I-00161 Roma, Italy.
Proc Natl Acad Sci U S A. 2022 Feb 22;119(8). doi: 10.1073/pnas.2119288119.
We study the instantaneous normal mode (INM) spectrum of a simulated soft-sphere liquid at different equilibrium temperatures We find that the spectrum of eigenvalues [Formula: see text] has a sharp maximum near (but not at) [Formula: see text] and decreases monotonically with [Formula: see text] on both the stable and unstable sides of the spectrum. The spectral shape strongly depends on temperature. It is rather asymmetric at low temperatures (close to the dynamical critical temperature) and becomes symmetric at high temperatures. To explain these findings we present a mean-field theory for [Formula: see text], which is based on a heterogeneous elasticity model, in which the local shear moduli exhibit spatial fluctuations, including negative values. We find good agreement between the simulation data and the model calculations, done with the help of the self-consistent Born approximation (SCBA), when we take the variance of the fluctuations to be proportional to the temperature More importantly, we find an empirical correlation of the positions of the maxima of [Formula: see text] with the low-frequency exponent of the density of the vibrational modes of the glasses obtained by quenching to [Formula: see text] from the temperature We discuss the present findings in connection to the liquid to glass transformation and its precursor phenomena.
我们研究了在不同平衡温度下模拟软球液体的瞬时正常模式(INM)谱。我们发现,本征值谱[公式:见正文]在[公式:见正文]附近(但不在该点)有一个尖锐的最大值,并且在谱的稳定和不稳定两侧都随[公式:见正文]单调下降。谱的形状强烈依赖于温度。在低温(接近动力学临界温度)时它相当不对称,而在高温时变得对称。为了解释这些发现,我们提出了一种关于[公式:见正文]的平均场理论,该理论基于一种非均匀弹性模型,其中局部剪切模量表现出空间涨落,包括负值。当我们将涨落的方差取为与温度成比例时,我们发现模拟数据与借助自洽玻恩近似(SCBA)进行的模型计算之间有很好的一致性。更重要的是,我们发现[公式:见正文]最大值位置与通过从温度淬火到[公式:见正文]得到的玻璃振动模式密度的低频指数之间存在经验相关性。我们结合液体到玻璃的转变及其前驱现象讨论了当前的发现。