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We present a bias-controlled spin-filtering mechanism in spin-valves including a hybrid organic chain/graphene interface. Wet growth conditions of oligomeric molecular chains would usually lead, during standard CMOS-compatible fabrication processes, to the quenching of spintronics properties of metallic spin sources due to oxidation. We demonstrate by X-ray photoelectron spectroscopy that the use of a protective graphene layer fully preserves the metallic character of the ferromagnetic surface and thus its capability to deliver spin polarized currents. We focus here on a small aromatic chain of controllable lengths, formed by nitrobenzene monomers and derived from the commercial 4-nitrobenzene diazonium tetrafluoroborate, covalently attached to the graphene passivated spin sources thanks to electroreduction. A unique bias dependent switch of the spin signal is then observed in complete spin valve devices, from minority to majority spin carriers filtering. First-principles calculations are used to highlight the key role played by the spin-dependent hybridization of electronic states present at the different interfaces. Our work is a first step towards the exploration of spin transport using different functional molecular chains. It opens the perspective of atomic tailoring of magnetic junction devices towards spin and quantum transport control, thanks to the flexibility of ambient electrochemical surface functionalization processes.

van der Waals atomically thin magnetic materials have been recently discovered. They have attracted enormous attention as they present unique magnetic properties, holding potential to tailor spin-based device properties and enable next generation data storage and communication devices. To fully understand the magnetism in two-dimensions, the synthesis of 2D materials over large areas with precise thickness control has to be accomplished. Here, we review the recent advancements in the synthesis of these materials spanning from metal halides, transition metal dichalcogenides, metal phosphosulphides, to ternary metal tellurides. We initially discuss the emerging device concepts based on magnetic van der Waals materials including what has been achieved with graphene. We then review the state of the art of the synthesis of these materials and we discuss the potential routes to achieve the synthesis of wafer-scale atomically thin magnetic materials. We discuss the synthetic achievements in relation to the structural characteristics of the materials and we scrutinise the physical properties of the precursors in relation to the synthesis conditions. We highlight the challenges related to the synthesis of 2D magnets and we provide a perspective for possible advancement of available synthesis methods to respond to the need for scalable production and high materials quality.