Ab initio energies of nonconducting crystals by systematic fragmentation

摘要

A systematic method for approximating the ab initio electronic energy of molecules from the energies of molecular fragments has been adapted to estimate the total electronic energy of crystal lattices.The fragmentation method can be employed with any ab initio electronic structure method and allows optimization of the crystal structure based on ab initio gradients.The method is demonstrated on SiO2 polymorphs using the Hartree-Fock approximation,second order Moller-Plesset perturbation theory,and the quadratic configuration interaction method with single and double excitations and triple excitations added perturbatively.