Wigner-molecule supercrystal in transition-metal dichalcogenide moir\'e superlattices: Lessons from the bottom-up approach

The few-body problem for $N=4$ fermionic charge carriers in a double-well moir\'{e} quantum dot (MQD), representing the first step in a bottom-up strategy to investigate formation of molecular supercrystals in transition metal dichalcogenide (TMD) moir\'e superlattices with integral fillings, $\nu > 1$, is solved exactly by employing large-scale exact-diagonalization via full configuration interaction (FCI) computations. A comparative analysis with the mean-field solutions of the often used spin-and-space unrestricted Hartree Fock (sS-UHF) demonstrates the limitations of the UHF method (by itself) to provide a proper description of the influence of the interdot Coulomb interaction. In particular, it is explicitly shown for $\nu=2$ that the exact charge densities (CDs) within each MQD retain the ring-like shape characteristic (for a wide range of relevant parameters) of a fully isolated MQD, as was found for sliding Wigner molecules (WMs). This deeply quantum-mechanical behavior contrasts sharply with the UHF CDs that portray solely orientationally pinned and well localized dumbbell dimers. An improved CD, which agrees with the FCI-calculated one, derived from the restoration of the sS-UHF broken parity symmetries is further introduced, suggesting a beyond-mean-field methodological roadmap for correcting the sS-UHF results. It is conjectured that the conclusions for the $\nu=2$ moir\'e TMD superlattice case extend to all cases with integral fillings that are associated with sliding WMs in isolated MQDs. The case of $\nu=3$, associated with a pinned WM in isolated MQDs, is an exception.
Comment: 9-page Letter with 5 color figures. For related papers, see https://sites.gatech.edu/cyannouleas/