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Register a new userElectrically addressing the spin of a magnetic porphyrin through covalently connected graphene electrodes
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We report on the fabrication and transport characterization of atomically-precise single molecule devices consisting of a magnetic porphyrin covalently wired by graphene nanoribbon electrodes. The tip of a scanning tunneling microscope was utilized to contact the end of a GNR-porphyrin-GNR hybrid system and create a molecular bridge between tip and sample for transport measurements. Electrons tunneling through the suspended molecular heterostructure excited the spin multiplet of the magnetic porphyrin. The detachment of certain spin-centers from the surface shifted their spin-carrying orbitals away from an on-surface mixed-valence configuration, recovering its original spin state. The existence of spin-polarized resonances in the free-standing systems and their electrical addressability is the fundamental step for utilization of carbon-based materials as functional molecular spintronics systems.
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Graphene is expected to complement todays Si-based information technology. In particular, magnetic molecules in contact with graphene constitute a tantalizing approach towards organic spin electronics because of the reduced conductivity mismatch at the interface. In such a system a bit is represented by a single molecular magnetic moment, which must be stabilized against thermal fluctuations. Here, we show in a combined experimental and theoretical study that the moments of paramagnetic Co-octaethylporphyrin (CoOEP) molecules on graphene can be aligned by a remarkable antiferromagnetic coupling to a Ni substrate underneath the graphene. This coupling is mediated via the pi electronic system of graphene, while no covalent bonds between the molecule and the substrate are established.
Scattering of electrons by localized spins is the ultimate process enabling electrical detection and control of the magnetic state of a spin-doped material. At the molecular scale, this scattering is mediated by the electronic orbitals hosting the spin. Here we report the selective excitation of a molecular spin by electrons tunneling through different molecular orbitals. Spatially-resolved tunneling spectra on iron porphyrins on Au(111) reveal that the inelastic spin excitation extends beyond the iron site. The inelastic features also change shape and symmetry along the molecule. Combining DFT simulations with a phenomenological scattering model, we show that the extension and lineshape variations of the inelastic signal are due to excitation pathways assisted by different frontier orbitals, each of them with a different degree of hybridization with the surface. By selecting the intramolecular site for electron injection, the relative weight of iron and pyrrole orbitals in the tunneling process is modified. In this way, the spin excitation mechanism, reflected by its spectral lineshape, changes depending on the degree of localization and energy alignment of the chosen molecular orbital.
Using density-functional calculations, we study the effect of sp$^3$-type defects created by different covalent functionalizations on the electronic and magnetic properties of graphene. We find that the induced magnetic properties are {it universal}, in the sense that they are largely independent on the particular adsorbates considered. When a weakly-polar single covalent bond is established with the layer, a local spin-moment of 1.0 $mu_B$ always appears in graphene. This effect is similar to that of H adsorption, which saturates one $p_z$ orbital in the carbon layer. The magnetic couplings between the adsorbates show a strong dependence on the graphene sublattice of chemisorption. Molecules adsorbed at the same sublattice couple ferromagnetically, with an exchange interaction that decays very slowly with distance, while no magnetism is found for adsorbates at opposite sublattices. Similar magnetic properties are obtained if several $p_z$ orbitals are saturated simultaneously by the adsorption of a large molecule. These results might open new routes to engineer the magnetic properties of graphene derivatives by chemical means.
In graphene spintronics, interaction of localized magnetic moments with the electron spins paves a new way to explore the underlying spin relaxation mechanism. A self-assembled layer of organic cobalt-porphyrin (CoPP) molecules on graphene provides a desired platform for such studies via the magnetic moments of porphyrin-bound cobalt atoms. In this work a study of spin transport properties of graphene spin-valve devices functionalized with such CoPP molecules as a function of temperature via non-local spin-valve and Hanle spin precession measurements is reported. For the functionalized (molecular) devices, we observe a slight decrease in the spin relaxation time ({tau}s), which could be an indication of enhanced spin-flip scattering of the electron spins in graphene in the presence of the molecular magnetic moments. The effect of the molecular layer is masked for low quality samples (low mobility), possibly due to dominance of Elliot-Yafet (EY) type spin relaxation mechanisms.
We theoretically study the spin-polarized transport through a single-molecule magnet, which is weakly coupled to ferromagnetic leads, by means of the rate-equation approach. We consider both the ferromagnetic and antiferromagnetic exchange-couplings between the molecular magnet and transported electron-spin in the nonlinear tunneling regime. For the ferromagnetic exchangecoupling, spin current exhibits step- and basin-like behaviors in the parallel and antiparallel configurations respectively. An interesting observation is that the polarization reversal of spin-current can be realized and manipulated by the variation of bias voltage in the case of antiferromagnetic exchange-coupling with antiparallel lead-configuration, which may be useful in the development of spintronic devices, while the bias voltage can only affect the magnitude of spin-polarization in the ferromagnetic coupling.
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