Downfolding electron-phonon Hamiltonians from ab-initio calculations: application to K$_3$Picene

TL;DR

This paper introduces a method to derive accurate electron-phonon Hamiltonians from ab-initio calculations, incorporating a double-counting correction, and applies it to potassium-doped picene to study its electronic properties.

Contribution

It presents a novel parameterization technique for electron-phonon models that includes a double-counting correction, validated on K3Picene from first-principles data.

Findings

The system remains an insulator despite strong electron-phonon coupling.

The Hubbard repulsion dominates, leading to a small Mott gap.

The method accurately reproduces system geometry and vibrational frequencies.

Abstract

We propose an electron-phonon parameterization which reliably reproduces the geometry and harmonic frequencies of a real system. With respect to standard electron-phonon models, it adds a "double-counting" correction, which takes into account the lattice deformation as the system is dressed by low-energy electron-phonon processes. We show the importance of this correction by studying potassium-doped picene (K$_3$Picene), recently claimed to be a superconductor with a $T_c$ of up to 18 K. The Hamiltonian parameters are derived from ab-initio density functional theory, and the lattice model is solved by dynamical mean-field theory. Our calculations include the effects of electron-electron interactions and local electron-phonon couplings. Even with the inclusion of a strongly coupled molecular phonon, the Hubbard repulsion prevails and the system is an insulator with a small Mott gap of $\approx$ 0.2 eV.