Department of Physics and Astronomy, University of Pennsylvania, Philadelphia Pennsylvania 19104, USA.
J Chem Phys. 2013 Mar 28;138(12):12A525. doi: 10.1063/1.4774076.
We study connections between vibrational spectra and average nearest neighbor number in disordered clusters of colloidal particles with attractive interactions. Measurements of displacement covariances between particles in each cluster permit calculation of the stiffness matrix, which contains effective spring constants linking pairs of particles. From the cluster stiffness matrix, we derive vibrational properties of corresponding "shadow" glassy clusters, with the same geometric configuration and interactions as the "source" cluster but without damping. Here, we investigate the stiffness matrix to elucidate the origin of the correlations between the median frequency of cluster vibrational modes and average number of nearest neighbors in the cluster. We find that the mean confining stiffness of particles in a cluster, i.e., the ensemble-averaged sum of nearest neighbor spring constants, correlates strongly with average nearest neighbor number, and even more strongly with median frequency. Further, we find that the average oscillation frequency of an individual particle is set by the total stiffness of its nearest neighbor bonds; this average frequency increases as the square root of the nearest neighbor bond stiffness, in a manner similar to the simple harmonic oscillator.
我们研究了具有吸引力相互作用的胶体粒子无序团簇中振动谱与平均最近邻数之间的关系。对每个团簇中粒子的位移协方差进行测量,可计算出僵硬矩阵,其中包含连接粒子对的有效弹簧常数。从团簇僵硬矩阵,我们推导出相应的“阴影”玻璃状团簇的振动特性,其具有与“源”团簇相同的几何构型和相互作用,但没有阻尼。在这里,我们研究了僵硬矩阵,以阐明团簇振动模式的中值频率与团簇中最近邻数之间的相关性的起源。我们发现,团簇中粒子的平均约束刚度,即最近邻弹簧常数的集合平均值,与平均最近邻数强烈相关,与中值频率的相关性更强。此外,我们发现单个粒子的平均振荡频率由其最近邻键的总刚度决定;这种平均频率随最近邻键刚度的平方根增加,类似于简谐振荡器。