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Quasicrystalline materials exhibit long-range order but no translational periodicity. Now, a random tiling quasicrystal has been fabricated on a Au(111) surface by coordination interactions between europium centres and linear dicarbonitrile linkers under stoichiometry control. The 2D metal–organic network exhibits the simultaneous presence of four-, five- and six-fold vertices and dodecagonal symmetry.

It is challenging to determine thermodynamic quantities for single molecules. Here, the authors access single-molecule thermodynamic information via a microscopic and computational study of a confined molecule, for which the resulting patterns represent a real-space equilibrium probability distribution.

Understanding cycloaddition mechanisms is beneficial for the creation of extended carbon nanostructures, yet traditional models often overlook symmetry-based mechanistic effects. Here, the authors employ topological classifiers to identify symmetry-forbidden pathways in polycyclic aromatic azomethine ylide cycloadditions, revealing that topologically-allowed endothermic reactions can guide nanographene engineering.

Topological phonon boundary modes (TBM) hold promises for advanced phononic applications. Here, the authors introduce the bulk-heavy boundary correspondence to pattern TBM in polymers and supramolecular assemblies under thermal fluctuations.

Graphene nanostructures with π magnetism offer a chemically tunable platform to explore correlated magnetic interactions. Here, the on-surface synthesis of spin-1/2 antiferromagnetic Heisenberg chains based on N-doped nanographene units is reported. The spin chains are synthesized through ortho sp³ C–H activated polymerization and exhibit parity-dependent magnetic ground states.

Two-dimensional, self-assembled heteromolecular networks often lack functionality. Here the authors study the photoresponse of self-assembled heteromolecular networks, while controlling their positions and interfaces at an atomic level, suggesting bottom-up assembly of optoelectronics devices.

The bottom-up fabrication of structures with robust performance in the nm-to-μm scale usable for integrated carbon nanodevices is challenging. Here the authors report micrometer-long, highly conducting nanographene wires following self-assembly, photo-crosslinking and thermal annealing of anthracene derivatives on hexagonal boron nitride sheets.

A critical milestone for the advancement of nanoscale organic circuitry is the fabrication of well-defined conjugated polymers on non-metal substrates. Here, the authors demonstrate extended polycyclic aromatic chains from repetitive cycloadditions which form not only on metals, but also on boron nitride layers and in the solid state.

Selective activation of C–H bonds is a key challenge in organic reactions. Here, the authors achieve the selective activation of four quasi-equivalent C–H bonds, leading to the formation of N-doped graphene nanoribbons with partial corannulene motifs.

Polyaromatic hydrocarbons can be precisely manipulated to yield ever more complex and discrete graphene analogs, such as nanographenes. Here, the authors use azomethine ylide homocoupling to insert an antiaromatic pyrazine ring into the core of a nanographene, and characterize the molecule’s unique electronic character.

The efficient engineering of nanostructures with semiconducting properties is vital to the development of organic electronics. This Perspective discusses a variety of techniques for fabricating such macromolecules, including graphene carving, the stimulus-induced synthesis of conjugated polymers and surface-assisted synthesis, and considers their potential for reproducing chemically and spatially precise molecular arrangements, that is 'molecular blueprints'.