Visualizing designer quantum states in stable macrocycle quantum corrals.

ABSTRACT

Creating atomically precise quantum architectures with high digital fidelity and desired quantum states is an important goal in a new era of quantum technology. The strategy of creating these quantum nanostructures mainly relies on atom-by-atom, molecule-by-molecule manipulation or molecular assembly through non-covalent interactions, which thus lack sufficient chemical robustness required for on-chip quantum device operation at elevated temperature. Here, we report a bottom-up synthesis of covalently linked organic quantum corrals (OQCs) with atomic precision to induce the formation of topology-controlled quantum resonance states, arising from a collective interference of scattered electron waves inside the quantum nanocavities. Individual OQCs host a series of atomic orbital-like resonance states whose orbital hybridization into artificial homo-diatomic and hetero-diatomic molecular-like resonance states can be constructed in Cassini oval-shaped OQCs with desired topologies corroborated by joint ab initio and analytic calculations. Our studies open up a new avenue to fabricate covalently linked large-sized OQCs with atomic precision to engineer desired quantum states with high chemical robustness and digital fidelity for future practical applications.