Ab initio pseudopotentials can in principle reproduce the scattering properties of the all-electron core at a finite set of arbitrarily chosen energies, but the faithful description of high-energy scattering states is often hindered by practical limitations and ill-conditioning. We present a novel approach for generating first-principles dynamical pseudopotentials, in which the flexibility of an energy-dependent construction is exploited to systematically improve transferability at the level of accuracy of density-functional theory. We first show that this energy dependence generalizes the norm-conservation condition [1], introducing soft pseudo-orbitals [2] and dynamical augmentation charges related to the derivative of the pseudopotential. We then introduce an effective embedding scheme to build pseudopotentials within a sum-over poles representation, enabling efficient electronic-structure calculations in conjunction with the algorithmic-inversion method for the exact solution of the Dyson equation [3,4]. Notably, the number of projectors in the nonlocal pseudopotential is disentangled from the number of reference energies at which scattering properties are reproduced, allowing for a systematic improvement of transferability without sacrificing numerical efficiency.
Laboratory for Materials Simulations (LMS)