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Strain-Tunable Spin Moment in Ni-Doped Graphene

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 Publication date 2011
  fields Physics
and research's language is English




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Graphene, due to its exceptional properties, is a promising material for nanotechnology applications. In this context, the ability to tune the properties of graphene-based materials and devices with the incorporation of defects and impurities can be of extraordinary importance. Here we investigate the effect of uniaxial tensile strain on the electronic and magnetic properties of graphene doped with substitutional Ni impurities (Ni_sub). We have found that, although Ni_sub defects are non-magnetic in the relaxed layer, uniaxial strain induces a spin moment in the system. The spin moment increases with the applied strain up to values of 0.3-0.4 mu_B per Ni_sub, until a critical strain of ~6.5% is reached. At this point, a sharp transition to a high-spin state (~1.9 mu_B) is observed. This magnetoelastic effect could be utilized to design strain-tunable spin devices based on Ni-doped graphene.



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Strain engineering of graphene takes advantage of one of the most dramatic responses of Dirac electrons enabling their manipulation via strain-induced pseudo-magnetic fields. Numerous theoretically proposed devices, such as resonant cavities and valley filters, as well as novel phenomena, such as snake states, could potentially be enabled via this effect. These proposals, however, require strong, spatially oscillating magnetic fields while to date only the generation and effects of pseudo-gauge fields which vary at a length scale much larger than the magnetic length have been reported. Here we create a periodic pseudo-gauge field profile using periodic strain that varies at the length scale comparable to the magnetic length and study its effects on Dirac electrons. A periodic strain profile is achieved by pulling on graphene with extreme (>10%) strain and forming nanoscale ripples, akin to a plastic wrap pulled taut at its edges. Combining scanning tunneling microscopy and atomistic calculations, we find that spatially oscillating strain results in a new quantization different from the familiar Landau quantization observed in previous studies. We also find that graphene ripples are characterized by large variations in carbon-carbon bond length, directly impacting the electronic coupling between atoms, which within a single ripple can be as different as in two different materials. The result is a single graphene sheet that effectively acts as an electronic superlattice. Our results thus also establish a novel approach to synthesize an effective 2D lateral heterostructure - by periodic modulation of lattice strain.
We report the discovery of a strong and tunable spin lifetime anisotropy with excellent spin lifetimes up to 7.8 ns in dual-gated bilayer graphene. Remarkably, this realizes the manipulation of spins in graphene by electrically-controlled spin-orbit fields, which is unexpected due to graphenes weak intrinsic spin-orbit coupling. We utilize both the in-plane magnetic field Hanle precession and oblique Hanle precession measurements to directly compare the lifetimes of out-of-plane vs. in-plane spins. We find that near the charge neutrality point, the application of a perpendicular electric field opens a band gap and generates an out-of-plane spin-orbit field that stabilizes out-of-plane spins against spin relaxation, leading to a large spin lifetime anisotropy. This intriguing behavior occurs because of the unique spin-valley coupled band structure of bilayer graphene. Our results demonstrate the potential for highly tunable spintronic devices based on dual-gated 2D materials.
Hydrogen adatoms are shown to generate magnetic moments inside single layer graphene. Spin transport measurements on graphene spin valves exhibit a dip in the non-local spin signal as a function of applied magnetic field, which is due to scattering (relaxation) of pure spin currents by exchange coupling to the magnetic moments. Furthermore, Hanle spin precession measurements indicate the presence of an exchange field generated by the magnetic moments. The entire experiment including spin transport is performed in an ultrahigh vacuum chamber, and the characteristic signatures of magnetic moment formation appear only after hydrogen adatoms are introduced. Lattice vacancies also demonstrate similar behavior indicating that the magnetic moment formation originates from pz-orbital defects.
Magnetic properties of graphenic carbon nanostructures, relevant for future spintronic applications, depend crucially on doping and on the presence of defects. In this paper we study the magnetism of the recently detected substitutional Ni (Ni(sub)) impurities. Ni(sub) defects are non-magnetic in flat graphene and develop a non-zero magnetic moment only in metallic nanotubes. This surprising behavior stems from the peculiar curvature dependence of the electronic structure of Ni(sub). A similar magnetic/non-magnetic transition of Ni(sub) can be expected by applying anisotropic strain to a flat graphene layer.
Graphene is a model system for the study of electrons confined to a strictly two-dimensional layer1 and a large number of electronic phenomena have been demonstrated in graphene, from the fractional2, 3 quantum Hall effect to superconductivity4. However, the coupling of conduction electrons to local magnetic moments5, 6, a central problem of condensed matter physics, has not been realized in graphene, and, given carbons lack of d or f electrons, magnetism in graphene would seem unlikely. Nonetheless, magnetism in graphitic carbon in the absence of transition-metal elements has been reported7-10, with explanations ranging from lattice defects11 to edge structures12, 13 to negative curvature regions of the graphene sheet14. Recent experiments suggest that correlated defects in highly-ordered pyrolytic graphite (HOPG) induced by proton irradiation9 or native to grain boundaries7, can give rise to ferromagnetism. Here we show that point defects (vacancies) in graphene15 are local moments which interact strongly with the conduction electrons through the Kondo effect6, 16-18 providing strong evidence that defects in graphene are indeed magnetic. The Kondo temperature TK is tunable with carrier density from 30-90 K; the high TK is a direct consequence of strong coupling of defects to conduction electrons in a Dirac material18. The results indicate that defect engineering in graphene could be used to generate and control carrier-mediated magnetism, and realize all-carbon spintronic devices. Furthermore, graphene should be an ideal system in which to probe Kondo physics in a widely tunable electron system.
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