Spin excitations in nanographene-based antiferromagnetic spin-1/2 Heisenberg chains

Antiferromagnetic Heisenberg chains exhibit two distinct types of excitation spectrum: gapped for integer-spin chains and gapless for half-integer-spin chains. However, in finite-length half-integer-spin chains, quantization induces a gap, requiring precise control over sufficiently long chains to study its evolution. Here we create length-controlled spin-1/2 Heisenberg chains by covalently linking Olympicenes—Olympic-ring-shaped magnetic nanographenes. With large exchange interactions, tunable lengths and negligible magnetic anisotropy, this system is ideal for investigating length-dependent spin excitations, probed via inelastic electron tunnelling spectroscopy. We observe a power-law decay of the lowest excitation energy with length L, following a 1/L dependence in the large-L regime, consistent with theory. For L = 50, a V-shaped excitation continuum confirms a gapless behaviour in the thermodynamic limit. Additionally, low-bias current maps reveal the standing wave of a single spinon in odd-numbered chains. Our findings provide evidence for the realization of a one-dimensional analogue of a gapless spin liquid within an artificial graphene lattice.