Preferential antiferromagnetic coupling of vacancies in graphene on
  SiO_2: Electron spin resonance and scanning tunneling spectroscopy

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Abstract

Monolayer graphene grown by chemical vapor deposition and transferred to SiO_2 is used to introduce vacancies by Ar^+ ion bombardment at a kinetic energy of 50 eV. The density of defects visible in scanning tunneling microscopy (STM) is considerably lower than the ion fluence implying that most of the defects are single vacancies. The vacancies are characterized by scanning tunneling spectroscopy (STS) on graphene and HOPG exhibiting a peak close to the Fermi level. The peak persists after air exposure up to 180 min, albeit getting broader. After air exposure for less than 60 min, electron spin resonance (ESR) at 9.6 GHz is performed. For an ion flux of 10/nm^2, we find a signal corresponding to a g-factor of 2.001-2.003 and a spin density of 1-2 spins/nm^2. The ESR signal consists of a mixture of a Gaussian and a Lorentzian of equal weight exhibiting a width down to 0.17 mT, which, however, depends on details of the sample preparation. The g-factor anisotropy is about 0.02%. Temperature dependent measurements reveal antiferromagnetic correlations with a Curie-Weiss temperature of -10 K. Albeit the electrical conductivity of graphene is significantly reduced by ion bombardment, the spin resonance induced change in conductivity is below 10^{-5}.

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Half-Metallic Graphene Nanoribbons

Young-Woo Son, Marvin L. Cohen, Steven Louie (2006)

Electrical current can be completely spin polarized in a class of materials known as half-metals, as a result of the coexistence of metallic nature for electrons with one spin orientation and insulating for electrons with the other. Such asymmetric electronic states for the different spins have been predicted for some ferromagnetic metals - for example, the Heusler compounds- and were first observed in a manganese perovskite. In view of the potential for use of this property in realizing spin-based electronics, substantial efforts have been made to search for half-metallic materials. However, organic materials have hardly been investigated in this context even though carbon-based nanostructures hold significant promise for future electronic device. Here we predict half-metallicity in nanometre-scale graphene ribbons by using first-principles calculations. We show that this phenomenon is realizable if in-plane homogeneous electric fields are applied across the zigzag-shaped edges of the graphene nanoribbons, and that their magnetic property can be controlled by the external electric fields. The results are not only of scientific interests in the interplay between electric fields and electronic spin degree of freedom in solids but may also open a new path to explore spintronics at nanometre scale, based on graphene.

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Spin-half paramagnetism in graphene induced by point defects

A. V. Krasheninnikov, R. Nair, M Sepioni … (2011)

Using magnetization measurements, we show that point defects in graphene - fluorine adatoms and irradiation defects (vacancies) - carry magnetic moments with spin 1/2. Both types of defects lead to notable paramagnetism but no magnetic ordering could be detected down to liquid helium temperatures. The induced paramagnetism dominates graphene's low-temperature magnetic properties despite the fact that maximum response we could achieve was limited to one moment per approximately 1000 carbon atoms. This limitation is explained by clustering of adatoms and, for the case of vacancies, by losing graphene's structural stability.

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Room-temperature ferromagnetism in graphite driven by 2D networks of point defects

C Flipse, M. I. Katsnelson, J Cervenka (2009)

Ferromagnetism in carbon-based materials is appealing for both applications and fundamental science purposes because carbon is a light and bio-compatible material that contains only s and p electrons in contrast to traditional ferromagnets based on 3d or 4f electrons. Here we demonstrate direct evidence for ferromagnetic order locally at defect structures in highly oriented pyrolytic graphite (HOPG) with magnetic force microscopy and in bulk magnetization measurements at room temperature. Magnetic impurities have been excluded as the origin of the magnetic signal after careful analysis supporting an intrinsic magnetic behavior of carbon. The observed ferromagnetism has been attributed to originate from unpaired electron spins localized at grain boundaries of HOPG. Grain boundaries form two-dimensional arrays of point defects, where their spacing depends on the mutual orientation of two grains. Depending on the distance between these point defects, scanning tunneling spectroscopy of grain boundaries showed two intense split localized states for small distances between defects ( 4 nm).