Tunable topological phases in nanographene-based spin-1/2 alternating-exchange Heisenberg chains

Unlocking the potential of topological order in many-body spin systems has been a key goal in quantum materials research. Despite extensive efforts, the quest for a versatile platform enabling site-selective spin manipulation, essential for tuning and probing diverse topological phases, has persisted. Here we utilize on-surface synthesis to construct spin-1/2 alternating-exchange Heisenberg chains by covalently linking Clar’s goblets—nanographenes each hosting two antiferromagnetically coupled spins. Using scanning tunnelling microscopy, we exert atomic-scale control over chain lengths, parities and exchange-coupling terminations, and probe their magnetic response via inelastic tunnelling spectroscopy. Our investigation confirms the gapped nature of bulk excitations in the chains, known as triplons. Their dispersion relation is extracted from the spatial variation of tunnelling spectral amplitudes. Depending on the parity and termination of chains, we observe varying numbers of in-gap spin-1/2 edge excitations, reflecting the degeneracy of distinct topological ground states in the thermodynamic limit. By monitoring interactions between these edge spins, we identify the exponential decay of spin correlations. Our findings present a phase-controlled many-body platform, opening avenues toward spin-based quantum devices. Scanning probe microscopy experiments realize the alternating-exchange spin-1/2 Heisenberg model via magnetic nanographene chains. They control odd- to even-Haldane phase transitions and monitor spin–spin correlations and triplon dispersion.