No Arabic abstract
Understanding the coupling of graphene with its local environment is critical to be able to integrate it in tomorrows electronic devices. Here we show how the presence of a metallic substrate affects the properties of an atomically tailored graphene layer. We have deliberately introduced single carbon vacancies on a graphene monolayer grown on a Pt(111) surface and investigated its impact in the electronic, structural and magnetic properties of the graphene layer. Our low temperature scanning tunneling microscopy studies, complemented by density functional theory, show the existence of a broad electronic resonance above the Fermi energy associated with the vacancies. Vacancy sites become reactive leading to an increase of the coupling between the graphene layer and the metal substrate at these points; this gives rise to a rapid decay of the localized state and the quenching of the magnetic moment associated with carbon vacancies in free-standing graphene layers.
Spin-orbit splitting in graphene on Ni, Au, or Ag (111) substrates was examined on the basis of density-functional theory. Graphene grown on the three metals was found to have Rashba splitting of a few or several tens of meV. The strong splitting obtained on Au or Ag substrates was mainly ascribed to effective hybridization of graphene $p_{z}$ state with Au or Ag $d_{z^{2}}$ states, rather than charge transfer as previously proposed. Our work provides theoretical understandings of the metal-induced Rashba effect in graphene.
We investigate the electronic and magnetic properties of single Fe, Co, and Ni atoms and clusters on monolayer graphene (MLG) on SiC(0001) by means of scanning tunneling microscopy (STM), x-ray absorption spectroscopy, x-ray magnetic circular dichroism (XMCD), and ab initio calculations. STM reveals different adsorption sites for Ni and Co adatoms. XMCD proves Fe and Co adatoms to be paramagnetic and to exhibit an out-of-plane easy axis in agreement with theory. In contrast, we experimentally find a nonmagnetic ground state for Ni monomers while an increasing cluster size leads to sizeable magnetic moments. These observations are well reproduced by our calculations and reveal the importance of hybridization effects and intra-atomic charge transfer for the properties of adatoms and clusters on MLG.
Imperfections in the crystal structure, such as point defects, can strongly modify the optical and transport properties of materials. Here, we study the effect of point defects on the optical and DC conductivities of single layers of semiconducting transition metal dichalcogenides with the form $M$S$_2$, where $M$=Mo or W. The electronic structure is considered within a six bands tight-binding model, which accounts for the relevant combination of $d$ orbitals of the metal $M$ and $p$ orbitals of the chalcogen $S$. We use the Kubo formula for the calculation of the conductivity in samples with different distributions of disorder. We find that $M$ and/or S defects create mid-gap states that localize charge carriers around the defects and which modify the optical and transport properties of the material, in agreement with recent experiments. Furthermore, our results indicate a much higher mobility for $p$-doped WS$_2$ in comparison to MoS$_2$.
We perform ab initio calculations that indicate that the relative stability of antiphase boundaries (APB) with armchair and zigzag chiralities in monolayer boron nitride (BN) is determined by the chemical potentials of the boron and nitrogen species in the synthesis process. In an N-rich environment, a zigzag APB with N-rich core is the most stable structure, while under B-rich or intrinsic growth conditions, an armchair APB with stoichiometric core is the most stable. This stability transition is shown to arise from a competition between homopolar-bond (B-B and N-N) and elastic energy costs in the core of the APBs. Moreover, in the presence of a carbon source we find that a carbon-doped zigzag APB becomes the most stable boundary near the N-rich limit. The electronic structure of the two types of APBs in BN is shown to be particularly distinct, with the zigzag APB depicting defect-like deep electronic bands in the band gap, while the armchair APB shows bulk-like shallow electronic bands.
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.