Ab initio calculation of the refractive index and third-order nonlinear optical susceptibility of typical glass formers using the bond additivity model

摘要

We present an application of the bond additivity model to structural units of typical glass-forming materials with the use of ab initio molecular orbital theory. In order to estimate the refractive indices and third-order nonlinear optical susceptibilities of these materials, bond and reduced polarizabilities of the small cluster models are calculated on the basis of a localized molecular orbital analysis. The calculated refractive indices with local field correction well reproduce the experimental values while the calculated third-order optical susceptibilities are confined to showing the availability of this method for a qualitative nonlinear susceptibility estimation. This paper shows that if the effect of surface atoms is eliminated and the effect from the outside of the cluster is introduced appropriately, the macroscopic refractive indices can be derived from the microscopic bond polarizabilities by the calculation on even small cluster models.