4.8 Article

Ultrahigh-yield on-surface synthesis and assembly of circumcoronene into a chiral electronic Kagome-honeycomb lattice

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SCIENCE ADVANCES
卷 7, 期 3, 页码 -

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AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/sciadv.abf0269

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资金

  1. MOE [MOE2017-T2-1-056, MOE2019-T2-2-044, R-143-000-A75-11, R-143-000-B58-114]
  2. Czech Science Foundation [18-09914S]
  3. Praemium Academie of the Czech Academy of Sciences
  4. MEYS CR [LM2018110]
  5. NRF [NRF-NRFI05-2019-0005]
  6. MOE Tier 2 grant [MOE2018-T2-2-094]
  7. A*STAR under its AME YIRG grant [A20E6c0098]

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The study successfully achieved ultrahigh-yield synthesis of circumcoronene molecules on Cu(111) via surface-assisted intramolecular dehydrogenation, resulting in self-organization into an extended superlattice. The unique hexagonal zigzag topology of circumcoronenes and their nontrivial electronic properties on the metallic surface were revealed.
On-surface synthesis has revealed remarkable potential in the fabrication of atomically precise nanographenes. However, surface-assisted synthesis often involves multiple-step cascade reactions with competing pathways, leading to a limited yield of target nanographene products. Here, we devise a strategy for the ultrahigh-yield synthesis of circumcoronene molecules on Cu(111) via surface-assisted intramolecular dehydrogenation of the rationally designed precursor, followed by methyl radical-radical coupling and aromatization. An elegant electrostatic interaction between circumcoronenes and metallic surface drives their self-organization into an extended superlattice, as revealed by bond-resolved scanning probe microscopy measurements. Density functional theory and tight-binding calculations reveal that unique hexagonal zigzag topology of circumcoronenes, along with their periodic electrostatic landscape, confines two-dimensional electron gas in Cu(111) into a chiral electronic Kagome-honeycomb lattice with two emergent electronic flat bands. Our findings open up a new route for the high-yield fabrication of elusive nanographenes with zigzag topologies and their superlattices with possible nontrivial electronic properties.

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