In- and out-of-equilibrium {\em ab initio} theory of electrons and phonons

TL;DR

This paper develops a comprehensive ab initio many-body quantum theory for electrons and phonons in- and out-of-equilibrium, introducing a self-consistent Hamiltonian, deriving nonequilibrium Hedin and Kadanoff-Baym equations, and exploring conserving approximations.

Contribution

It presents the first ab initio derivation of nonequilibrium Green's function equations for electrons and phonons, including a self-consistent Hamiltonian and conserving approximations.

Findings

The Hamiltonian must be determined self-consistently to avoid inconsistencies.

The derived equations ensure conservation laws during time evolution.

Dynamical treatment of electron-phonon interactions can lead to phonon dispersion splitting.

Abstract

We lay down the {\em ab initio} many-body quantum theory of electrons and phonons in- and out-of-equilibrium at any temperature. We begin by addressing a fundamental issue concerning the {\em ab initio} Hamiltonian in the harmonic approximation, which we show must be determined {\em self-consistently} to avoid inconsistencies. After identifying the most suitable partitioning into a ``noninteracting'' and an ``interacting'' part we embark on the Green's function diagrammatic analysis. We single out key diagrammatic structures to carry on the expansion in terms of dressed propagators and screened interaction. The final outcome is the finite-temperature nonequilibrium extension of the Hedin equations, featuring the appearance of the time-local Ehrenfest diagram in the electronic self-energy. The Hedin equations have limited practical utility for real-time simulations of driven systems. We leverage the versatility of diagrammatic expansion to generate a closed system of integro-differential equations for the Green's functions and nuclear displacements. These are the Kadanoff-Baym equations for electrons and phonons. Another advantage of the diagrammatic derivation is the ability to use conserving approximations, which ensure the satisfaction of all fundamental conservation laws during the time evolution. As an example we show that the adiabatic Born-Oppenheimer approximation is not conserving whereas its dynamical extension is conserving provided that the electrons are treated in the Fan-Migdal approximation with a dynamically screened electron-phonon coupling. We also derive the formal solution of the Kadanoff-Baym equations in the long time limit and at the steady state. The expansion of the phononic Green's function around the quasi-phonon energies points to a possible correlation-induced splitting of the phonon dispersion in materials with no time-reversal invariance.