No Arabic abstract
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.
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.
We present first principles calculations of the exchange interactions between magnetic impurities deposited on (001), (110) and (111) surfaces of Cu and Au and analyze them, in particular, in the asymptotic regime. For the (110) and the (111) surfaces we demonstrate that the interaction shows an oscillatory behavior as a function of the distance, R, of the impurities and that the amplitude of the oscillations decays as 1/R^2. Furthermore, the frequency of the oscillations is closely related to the length of the Fermi vector of the surface states existing on these surfaces. Due to the asymmetry of the the surface states dispersion, the frequency of the oscillations becomes also asymmetric on the (110) surfaces, while on the Au(111) surface two distinct frequencies are found in the oscillations as a consequence of the Bychkov-Rashba splitting of the surface states. Remarkably, no long range oscillations of the exchange interaction are observed for the (001) surfaces where the surface states are unoccupied. When burying the impurities beneath the surface layer, oscillations mediated by the bulk states become visible.
The electronic properties and optical excitations are investigated in the geometry- and field-modulated bilayer graphene systems, respectively, by using the tight-binding model and Kubo formula. The stacking symmetry of bilayer graphene can be manipulated by varying the width and position of domain wall (DW) within two normally stacked graphene. All the layer-dependent atomic interactions are taken into consideration under external fields. The modulation of stacking configuration gives rise to significant effects of zone folding on energy subbands, subenvelope wave functions, density of states, and optical absorption spectra. This study clearly illustrates the diverse 1D phenomena in the energy band structure and absorption spectra; the DW- and $V_z$-created dramatic variations are comprehensively explored under accurate calculations and delicate analysis. Concise physical pictures are proposed to give further insight into the quasi-1D behaviors.
We investigate the adsorption of graphene sheets on h-BN substrates by means of first-principles calculations in the framework of adiabatic connection fluctuation-dissipation theory in the random phase approximation. We obtain adhesion energies for different crystallographic stacking configurations and show that the interlayer bonding is due to long-range van der Waals forces. The interplay of elastic and adhesion energies is shown to lead to stacking disorder and moire structures. Band structure calculations reveal substrate induced mass terms in graphene which change their sign with the stacking configuration. The dispersion, absolute band gaps and the real space shape of the low energy electronic states in the moire structures are discussed. We find that the absolute band gaps in the moire structures are at least an order of magnitude smaller than the maximum local values of the mass term. Our results are in agreement with recent STM experiments.
We present a theoretical study using density functional calculations of the structural, electronic and magnetic properties of 3d transition metal, noble metal and Zn atoms interacting with carbon monovacancies in graphene. We pay special attention to the electronic and magnetic properties of these substitutional impurities and found that they can be fully understood using a simple model based on the hybridization between the states of the metal atom, particularly the d shell, and the defect levels associated with an unreconstructed D3h carbon vacancy. We identify three different regimes associated with the occupation of different carbon-metal hybridized electronic levels: (i) bonding states are completely filled for Sc and Ti, and these impurities are non-magnetic; (ii) the non-bonding d shell is partially occupied for V, Cr and Mn and, correspondingly, these impurties present large and localized spin moments; (iii) antibonding states with increasing carbon character are progressively filled for Co, Ni, the noble metals and Zn. The spin moments of these impurities oscillate between 0 and 1 Bohr magnetons and are increasingly delocalized. The substitutional Zn suffers a Jahn-Teller-like distortion from the C3v symmetry and, as a consequence, has a zero spin moment. Fe occupies a distinct position at the border between regimes (ii) and (iii) and shows a more complex behavior: while is non-magnetic at the level of GGA calculations, its spin moment can be switched on using GGA+U calculations with moderate values of the U parameter.