Controlling the dynamics of spins on surfaces is pivotal to the design of spintronic1 and quantum computing2 devices. Proposed schemes involve the interaction of spins with graphene to enable surface-state spintronics3,4, and electrical spin-manipulation4-11. However, the influence of the graphene environment on the spin systems has yet to be unraveled12. Here we explore the spin-graphene interaction by studying the classical and quantum dynamics of molecular magnets13 on graphene. While the static spin response remains unaltered, the quantum spin dynamics and associated selection rules are profoundly modulated. The couplings to graphene phonons, to other spins, and to Dirac fermions are quantified using a newly-developed model. Coupling to Dirac electrons introduces a dominant quantum-relaxation channel that, by driving the spins over Villain’s threshold, gives rise to fully-coherent, resonant spin tunneling. Our findings provide fundamental insight into the interaction between spins and graphene, establishing the basis for electrical spin-manipulation in graphene nanodevices.

We discuss current developments in the synthesis and characterization of magnetic nanohybrids made of molecular magnets and nanostructured materials. We first review several novel approaches that have recently been attempted to combine magnetic coordination complexes with differently-obtained inorganic systems. Special focus is placed on how the altered environment can affect the magnetic properties of single molecules, providing new routes to multifunctional devices based on hybrid magnetic nanosystems. We then show how this approach is opening new outlooks towards the control of nanomagnets using external stimuli (e.g. photons, electrons, etc.) and for the creation of ultra-sensitive devices. Eventually we provide a unified vision of the area, with a personal perspective on the main goals currently at stake and of possible future developments.

We show that individual, isolated graphene nanoribbons, created with a molecular synthetic approach, can be assembled on functionalised wafer surfaces treated with silanes. The use of surface groups with different hydrophobicities allows tuning the density of the ribbons and assessing the products of the polymerisation process.

Graphite is a clean substrate and its nanostructures hold great potential for applications. Anchoring large molecules on graphite represents a challenge for several reasons that essentially rise from the planar bonds of the packed honeycomb structure of carbon. Here, a systematic investigation by AFM and XPS on different derivatives of molecular Cr7Ni rings deposited on highly oriented pyrolytic graphite (HOPG) is reported. Cr7Ni is emerging as a prototipical example of molecular antiferromagnet on which quantum phenomena and coherence have been demonstrated. For the deposition of Cr7Ni on HOPG, two strategies are adopted: 1) Cr7Ni rings are functionalized with extended alkyl/benzene terminations and 2) a self‐assembled monolayer of alkyl chains with sulfonate terminations is deposited and then a cationic Cr7Ni derivative is used. In both cases the electronic bond with the carbon surface is soft, but the two‐step procedure is efficient, albeit indirect, in sticking molecular Cr7Ni on HOPG. These strategies can be easily extended to deposit other complex molecular aggregates on graphite from the liquid phase.