Visualizing designer quantum states in stable macrocycle quantum corrals

Xinnan Peng,Pingo Mutombo,Shaoqiang Dong,Mykola Telychko,Pei Wen Ng,Jiong Lu,Jishan Wu,Pavel Jelínek,Harshitra Mahalingam,Chunyan Chi,Aleksandr Rodin,Pin Lyu,Shaotang Song,Jie Su

doi:10.1038/s41467-021-26198-8

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.

Highlights

Creating atomically precise quantum architectures with high digital fidelity and desired quantum states is an important goal in a new era of quantum technology
Artificial quantum nanostructures created by these two methods do not have the sufficient chemical robustness required for practical applications
On-surface bottom-up synthesis has revealed its remarkable potential in the fabrication of atomically precise quantum architectures[22,23]

Summary

Introduction

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 synthesis of large-sized organic macrocycles requires delicate control over both thermodynamic and kinetic factors since competitive reaction pathways often yield different side products, and entropy effects disfavour the formation of the ordered rings[30,31,32] To this end, we have devised an on-surface synthetic protocol to construct atomically precise covalently linked OQCs from a well-designed organic precursor on Au(111), with the formation of a series of new quantum resonance states, arising from a collective interference of scattered electron waves inside the OQCs. By means of scanning tunneling microscopy, we have directly visualized multiple artificial atomic orbital-like resonance states hosted in individual OQCs, whose orbital hybridization into artificial homo-diatomic and hetero-diatomic molecular-like resonance states can be constructed in OQCs with desired topologies corroborated by joint ab initio and analytic calculations

Methods

Results

Conclusion