Precise control over the size and shape of graphene nanostructures allows engineering spin-polarized edge and topological states, representing a novel source of non-conventional π-magnetism with promising applications in quantum spintronics. A prerequisite for their emergence is the existence of robust gapped phases, which are difficult to find in extended graphene systems. Here we show that semi-metallic chiral GNRs (chGNRs) narrowed down to nanometer widths undergo a topological phase transition. We fabricated atomically precise chGNRs of different chirality and size by on surface synthesis using predesigned molecular precursors. Combining scanning tunneling microscopy (STM) measurements and theory simulations, we follow the evolution of topological properties and bulk band gap depending on the width, length, and chirality of chGNRs. Our findings represent a new platform for producing topologically protected spin states and demonstrate the potential of connecting chiral edge and defect structure with band engineering. Graphene nanoribbons are potential systems for engineering topological phases of matter, but the pre-required gapped phases are difficult to find. Here, the authors show that chiral graphene nanoribbons undergo a transition from metallic to topological insulators, and then to trivial band insulators as they are narrowed down to nanometer widths.

/pdf/topological-phase-transition-in-chiral-graphene-nanoribbons-2av1m0xd53.pdf

Topological phase transition in chiral graphene nanoribbons: from edge bands to end states.

Triangulene nanographenes are open-shell molecules with predicted high spin state due to the frustration of their conjugated network. Their long-sought synthesis became recently possible over a metal surface. Here, we present a macrocycle formed by six [3]triangulenes, which was obtained by combining the solution synthesis of a dimethylphenyl-anthracene cyclic hexamer and the on-surface cyclodehydrogenation of this precursor over a gold substrate. The resulting triangulene nanostar exhibits a collective spin state generated by the interaction of its 12 unpaired π-electrons along the conjugated lattice, corresponding to the antiferromagnetic ordering of six S=1 sites (one per triangulene unit). Inelastic electron tunneling spectroscopy resolved three spin excitations connecting the singlet ground state with triplet states. The nanostar behaves close to predictions from the Heisenberg model of an S=1 spin ring, representing a unique system to test collective spin modes in cyclic systems.

On-Surface Synthesis and Collective Spin Excitations of a Triangulene-Based Nanostar.

Low dimensional carbon-based materials can show intrinsic magnetism associated to p-electrons in open-shell π-conjugated systems. Chemical design provides atomically precise control of the π-electron cloud, which makes them promising for nanoscale magnetic devices. However, direct verification of their spatially resolved spin-moment remains elusive. Here, we report the spin-polarization of chiral graphene nanoribbons (one-dimensional strips of graphene with alternating zig-zag and arm-chair boundaries), obtained by means of spin-polarized scanning tunnelling microscopy. We extract the energy-dependent spin-moment distribution of spatially extended edge states with π-orbital character, thus beyond localized magnetic moments at radical or defective carbon sites. Guided by mean-field Hubbard calculations, we demonstrate that electron correlations are responsible for the spin-splitting of the electronic structure. Our versatile platform utilizes a ferromagnetic substrate that stabilizes the organic magnetic moments against thermal and quantum fluctuations, while being fully compatible with on-surface synthesis of the rapidly growing class of nanographenes. 

pdf/detecting-the-spin-polarization-of-edge-states-in-graphene-3jayej2cv1.pdf

Detecting the spin-polarization of edge states in graphene nanoribbons

Precise control over the size and shape of graphene nanostructures allows engineering spin-polarized edge and topological states, representing a novel source of non-conventional $\pi$-magnetism with promising applications in quantum spintronics. A prerequisite for their emergence is the existence of robust gapped phases, which are difficult to find in extended graphene systems: only armchair graphene nanoribbons (GNRs) show a band gap that, however, closes for any other GNR orientation. Here we show that semi-metallic chiral GNRs (chGNRs) narrowed down to nanometer widths undergoes a topological phase transition, becoming first topological insulators, and transforming then into trivial band insulators for the narrowest chGNRs. We fabricated atomically precise chGNRs of different chirality and size by on surface synthesis using predesigned molecular precursors. Combining scanning tunnelling microscopy (STM) measurements and theory simulations, we follow the evolution of topological properties and bulk band gap depending on the width, length, and chirality of chGNRs. The first emerging gapped phases are topological, protected by a chiral interaction pattern between edges. For narrower ribbons, the symmetry of the interaction pattern changes, and the topological gap closes and re-opens again as a trivial band insulator. Our findings represent a new platform for producing topologically protected spin states and demonstrates the potential of connecting chiral edge and defect structure with band engineering.

/pdf/topological-phase-transition-in-chiral-graphene-nanoribbons-raed5oapeb.pdf

Topological phase transition in chiral graphene nanoribbons: from edge bands to end states

Open-shell polycyclic aromatic hydrocarbons (PAHs) represent promising building blocks for carbon-based functional magnetic materials. Their magnetic properties stem from the presence of unpaired electrons localized in radical states of π character. Consequently, these materials are inclined to exhibit spin delocalization, form extended collective states, and respond to the flexibility of the molecular backbones. However, they are also highly reactive, requiring structural strategies to protect the radical states from reacting with the environment. Here, we demonstrate that the open-shell ground state of the diradical 

Tuning the Spin Interaction in Nonplanar Organic Diradicals through Mechanical Manipulation

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