All-electron magnetic response with pseudopotentials: NMR chemical shifts

Abstract

A theory for the ab initio calculation of all-electron NMR chemical shifts in insulators using pseudopotentials is presented. It is formulated for both finite and infinitely periodic systems and is based on an extension to the projector augmented-wave approach of Blöchl [P. E. Blöchl, Phys. Rev. B 50, 17 953 (1994)] and the method of Mauri et al. [F. Mauri, B. G. Pfrommer, and S. G. Louie, Phys. Rev. Lett. 77, 5300 (1996)]. The theory is successfully validated for molecules by comparison with a selection of quantum chemical results, and in periodic systems by comparison with plane-wave all-electron results for diamond.