Abstract
AbstractThe chemical functionalization of fullerene single molecule magnet Tb2@C80(CH2Ph) enables the facile preparation of robust monolayers on graphene and highly oriented pyrolytic graphite from solution without impairing their magnetic properties. Monolayers of endohedral fullerene functionalized with pyrene exhibit magnetic bistability up to a temperature of 28 K. The use of pyrene terminated linker molecules opens the way to devise integration of spin carrying units encapsulated by fullerene cages on graphitic substrates, be it single‐molecule magnets or qubit candidates.
Highlights
Introduction range up to80 K,[2] but the transfer of these properties from the bulk to nanoscale assemblies is lagging behind, and the mag-The realization of single-spin devices for magnetic memory or netic bistability of single-molecule magnets (SMMs) submonolayers is limited to 10 K at quantum information processing relies on the possibility to this moment.[3]create arrays of discrete magnetic units on suitable substrates, Here, we describe a breakthrough in the field of surfacewhich can function as device electrodes
Over a decade after the first observation of magnetic hysteresis in an Fe4 monolayer,[13] the temperature range in which this phenomenon could be observed for SMM monolayers expanded from sub-K regime to 10 K.[3b,c,f ] With this robust fullerene-based SMM, we make a major step forward and push the temperature range of the phenomenon to 28 K
This is comparable to Ho atoms on a thin layer of MgO|Ag(100), which demonstrate broad magnetic hysteresis up to 30 K[14] and magnetic bistability up to 45 K.[15]
Summary
The benzyl group on {Tb2}, which is needed for stabilization of the otherwise open-shell electronic structure, precludes the clean evaporation of the molecule onto surfaces. We concentrated on the deposition of {Tb2} onto graphene and graphite (HOPG). Known to show high affinity to graphitic substrates, was used to functionalize SMMs for their deposition on graphene and nanotubes in the past.[1b,6] To introduce pyrene groups to {Tb2}, we utilized the approach developed by Zaragoza-Galán et al.[7] for functionalization of. C60 with pyrene groups and used the derivative for subsequent SAM growth. The crude product of this dipolar cycloaddition reaction contained the targeted fulleropyrrolidine monoadduct bearing two pyrene groups, {Tb2}-pyr, along with unreacted educts and several other fulleropyrrolidine adducts. F,g) Laying-down and standing-up configurations of {Tb2}-pyr molecule on graphene from MD simulations, corresponding to mol 1 and mol 2 profiles in (e) at the time moment 120 ps. The analogous reaction was performed with Y2@C80(CH2Ph) ({Y2}) to obtain {Y2}-pyr
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