No Arabic abstract
We report a study of electronic transport in van der Waals heterostructures composed of flakes of the antiferromagnetic Mott insulator a-RuCl_3 placed on top of monolayer graphene Hall bars. While the zero-field transport shows a strong resemblance to that of isolated graphene, we find a consistently $p$-type Hall effect suggestive of multiband conduction, along with a non-monotonic and gate-voltage-dependent excursion of the resistivity at low temperatures that is reminiscent of transport in the presence of a magnetic phase transition. We interpret these data as evidence for charge transfer from graphene to a-RuCl_3 in an inhomogeneous device yielding both highly- and lightly-doped regions of graphene, while the latter shows a particular sensitivity to magnetism in the a-RuCl_3. Thus proximity to graphene is a means to access magnetic properties of thin layers of magnetic insulators.
By employing x-ray photoelectron spectroscopy (XPS), we have been able to establish the occurrence of charge-transfer doping in few-layer graphene covered with electron acceptor (TCNE) and donor (TTF) molecules. We have performed quantitative estimates of the extent of charge transfer in these complexes and elucidated the origin of unusual shifts of their Raman G bands and explained the differences in the dependence of conductivity on n- and p-doping. The study unravels the cause of the apparent difference between the charge-transfer doping and electrochemical doping.
At interfaces between conventional materials, band bending and alignment are classically controlled by differences in electrochemical potential. Applying this concept to oxides in which interfaces can be polar and cations may adopt a mixed valence has led to the discovery of novel two-dimensional states between simple band insulators such as LaAlO3 and SrTiO3. However, many oxides have a more complex electronic structure, with charge, orbital and/or spin orders arising from correlations between transition metal and oxygen ions. Strong correlations thus offer a rich playground to engineer functional interfaces but their compatibility with the classical band alignment picture remains an open question. Here we show that beyond differences in electron affinities and polar effects, a key parameter determining charge transfer at correlated oxide interfaces is the energy required to alter the covalence of the metaloxygen bond. Using the perovskite nickelate (RNiO3) family as a template, we probe charge reconstruction at interfaces with gadolinium titanate GdTiO3. X-ray absorption spectroscopy shows that the charge transfer is thwarted by hybridization effects tuned by the rare-earth (R) size. Charge transfer results in an induced ferromagnetic-like state in the nickelate, exemplifying the potential of correlated interfaces to design novel phases. Further, our work clarifies strategies to engineer two-dimensional systems through the control of both doping and covalence.
It is important to study the van der Waals interface in emerging vertical heterostructures based on layered two-dimensional (2D) materials. Being atomically thin, 2D materials are susceptible to significant strains as well as charge transfer doping across the interfaces. Here we use Raman and photoluminescence (PL) spectroscopy to study the interface between monolayer graphene/MoS2 heterostructures prepared by mechanical exfoliation and layer-by-layer transfer. By using correlation analysis between the Raman modes of graphene and MoS2 we show that both layers are subjected to compressive strain and charge transfer doping following mechanical exfoliation and thermal annealing. Furthermore, we show that both strain and carrier concentration can be modulated in the heterostructures with additional thermal annealing. Our study highlights the importance of considering both mechanical and electronic coupling when characterizing the interface in van der Waals heterostructures, and demonstrates a method to tune their electromechanical properties.
We perform Monte Carlo simulations to study the interplay of structural and magnetic order in single layer graphene covered with magnetic adatoms. We propose that the presence of ripples in the graphene structure can lead to clustering of the adatoms and to a variety of magnetic states such as super-paramagnetism, antiferromagnetism, ferromagnetism and spin glass behavior. We derive the magnetization hysteresis and also the magnetoresistance curves in the variable range hopping regime, which can provide experimental signatures for ripple induced clustering and magnetism. We propose that the magnetic states in graphene can be controlled by gate voltage and coverage fraction.
We predict that neutral graphene bilayers are pseudospin magnets in which the charge density-contribution from each valley and spin spontaneously shifts to one of the two layers. The band structure of this system is characterized by a momentum-space vortex which is responsible for unusual competition between band and kinetic energies leading to symmetry breaking in the vortex core. We discuss the possibility of realizing a pseudospin version of ferromagnetic metal spintronics in graphene bilayers based on hysteresis associated with this broken symmetry.