Abstract
On-surface synthesis has revealed remarkable potential in the fabrication of a plethora of
elusive nanographenes with tailored structural, electronic and magnetic properties
unattainable by conventional wet-chemistry synthesis. Unfortunately, surface-assisted
synthesis often involves multiple-step cascade reactions with competing pathways, leading
to the formation of a diversity of products with limited yield, which reduces its feasibility
towards the large-scale production for future technological applications. Here, we devise a
new on-surface synthetic strategy for the ultra-high yield synthesis of a hexagonal
nanographene with six zigzag edges, namely circumcoronene on Cu(111) via surfaceassisted intramolecular dehydrogenation of the rationally-designed precursor molecule,
followed by methyl radical-radical coupling and aromatization. An elegant electrostatic
interaction between circumcoronene and Cu(111) drives their self-organization into an
extended superlattice, as revealed by bond-resolved low-temperature scanning probe
microscopy and spectroscopy 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 (2D) electron gas in Cu(111)
surface into 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 novel 2D superlattices with possible nontrivial electronic properties towards their future technological applications.