Unifying dynamical electron-electron and electron-phonon interactions from first principles

Abstract

Electron-phonon interactions in materials with free carriers are dynamically screened by low-energy electronic excitations, yet first-principles calculations almost always treat this screening in the adiabatic approximation. A fully dynamical treatment of metals and doped semiconductors within time-dependent density functional perturbation theory (TDDFPT) is expensive and numerically delicate. Here, we introduce DFPT+A downfolding ("A" for active space), which starts from the static density functional perturbation theory (DFPT) response of a computationally convenient base system and adds the dynamical screening of a low-energy active space, described by Wannier functions. The required statically screened electron-electron interaction is computed using DFPT directly in the basis of Wannier-function pairs and truncated in a computationally efficient and systematically improvable way. The method handles entangled bands and accurately reproduces TDDFPT at a fraction of its cost. We use it to compute the total dynamical electron-electron interaction, including direct Coulomb and phonon-mediated interactions with dynamically screened electron-electron and electron-phonon couplings, all on equal footing. In hole-doped monolayer hBN, the hybridization of the carrier plasmon with the longitudinal optical phonon makes the low-energy retarded interaction nonmonotonic in the carrier density, an effect missed by the adiabatic approximation. In metallic monolayer TaS2, nonadiabatic effects are weak and occur only due to the intraband electron-hole continuum and the nesting of nearly parallel Fermi velocities. We also validate the widely used screened-screened approximation for the phonon spectral function. This work opens the way to first-principles studies of spectral functions, transport, and superconductivity with dynamically screened interactions.