RAW DATA for Detecting the spin-polarization of edge states in graphene nanoribbons

Low dimensional carbon-based materials can show intrinsic magnetism associated to p-electrons in open-shell $\pi$-conjugated systems. Chemical design provides atomically precise control of the $\pi$-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 $\pi$-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.