Ab initio lattice dynamics of nonconducting crystals by systematic fragmentation

Abstract

A systematic method for approximating the ab initio electronic energy of crystal lattices has been improved by the incorporation of long range electrostatic and dispersion interactions. The effect of these long range interactions on the optimization of the crystal structure is reported. The harmonic lattice dynamics have been evaluated to give phonon frequencies and neutron scattering intensities. Exemplary results are reported for diamond, silicon, and α-quartz using Hartree-Fock, Möller-Plesset perturbation, and coupled-cluster levels of ab initio theory.