Dynamical pseudopotentials for correlated-electron methods

First-principles pseudopotentials reproduce all-electron scattering at selected energies (typically, two); increasing this number is hindered by practical limitations and ill-conditioning.

We present a novel framework for generating pseudopotentials that are naturally dynamical and that can cover an arbitrary set of reference energies.

These pseudopotentials are also applicable to DFT, but naturally complement the dynamical self-energies that appear in GW, DMFT, or dynamical Hubbard approaches [1].

The energy dependence generalizes norm conservation, identifying dynamical augmentation charges related to the energy derivative of the pseudopotential.

Exploiting the algorithmic-inversion construction [1,2], we construct a sum-over poles pseudopotential by imposing norm-conservation in a system with augmented degrees of freedom, also decoupling the number of nonlocal projectors from the number of reference energies.

We demonstrate much improved transferability, reproducing the logarithmic derivative of Cu d-states up to 60 Ry, and we outline a stationary formulation of the total energy via a Klein functional, allowing for consistency with correlated-electron methods.

[1] T. Chiarotti, A. Ferretti and N. Marzari, Phys. Rev. Research 6, L032023 (2024)

[2] T. Chiarotti, N. Marzari and A. Ferretti, Phys. Rev. Research 4, 013242 (2022)