Atomistic hartree theory and crystal field of twisted double bilayer graphene near the magic angle

TL;DR

This study uses atomistic Hartree theory to analyze electron interactions and crystal field effects in twisted double bilayer graphene near the magic angle, revealing differences from previous DFT-based estimates and emphasizing screening effects.

Contribution

It provides a detailed atomistic Hartree analysis of electron-electron interactions and crystal field contributions in tDBLG, highlighting differences from prior DFT-based approaches.

Findings

Interactions do not cause significant doping-dependent band deformations in tDBLG.

Interactions screen the external electric field effectively.

Hartree-derived on-site energies are smaller but have the same sign as DFT-based estimates.

Abstract

Twisted double bilayer graphene (tDBLG) is a moir\'e material that has recently generated significant interest because of the observation of correlated phases near the magic angle. We carry out atomistic Hartree theory calculations to study the role of electron-electron interactions in the normal state. In contrast to twisted bilayer graphene (tBLG), we find that such interactions do not result in significant doping-dependent deformations of the electronic band structure. However, interactions play an important role for the electronic structure in the presence of a perpendicular electric field as they screen the external field. Finally, we analyze the contribution of the Hartree potential to the crystal field, i.e. the on-site energy difference between the inner and outer layers. We find that the on-site energy obtained from Hartree theory has the same sign, but a smaller magnitude compared to previous studies in which the on-site energy was determined by fitting tight-binding results to ab initio density-functional theory (DFT) band structures. To understand this quantitative difference, we analyze the ab initio Kohn-Sham potential obtained from DFT and find that a subtle interplay of electron-electron and electron-ion interactions determines the magnitude of the on-site potential.