Exciton Localization Modulated by Ultradeep Moiré Potential in Twisted Bilayer γ‑Graphdiyne

Twisted moiré superlattice is featured with its moiré potential energy, the depth of which renders an effective approach to strengthening the exciton–exciton interaction and exciton localization toward high-performance quantum photonic devices. However, it remains as a long-standing challenge to further push the limit of moiré potential depth. Herein, owing to the p z orbital induced band edge states enabled by the unique sp-C in bilayer γ-graphdiyne (GDY), an ultradeep moiré potential of ∼289 meV is yielded. After being twisted into the hole-to-hole layer stacking configuration, the interlayer coupling is substantially intensified to augment the lattice potential of bilayer GDY up to 475%. The presence of lateral constrained moiré potential shifts the spatial distribution of electrons and holes in excitons from the regular alternating mode to their respective separated and localized mode. According to the well-established wave function distribution of electrons contained in excitons, the AA-stacked site is identified to serve for exciton localization. This work extends the materials systems available for moiré superlattice design further to serial carbon allotropes featured with benzene ring-alkyne chain coupling, unlocking tremendous potential for twistronic-based quantum device applications.