Linking Vibrational Dynamics to Local Electronic Structure: Local Analysis of Dynamics of the relaxed Si$_{87}$ Cluster

Abstract

A flexible scheme for decomposing the vibrational density of states in terms of pair vibrational density of states is presented. This scheme provides the linkage between the site vibrational density of states and pair vibrational density of states so that vibrational modes, in particular localized modes, can be conveniently examined in terms of the correlation between the vibration at a given site and those at its neighboring sites. Furthermore, within the framework of a total energy vibrational spectrum study, this scheme allows the analysis of vibrational modes in terms of their electronic origin. A case study of the vibrational dynamics of the relaxed Si$_{87}$ cluster is carried out to demonstrate the flexibility of the scheme in analyzing the properties of vibrational modes, particularly for complex systems with reduced or no symmetry.