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Register a new userOn the structure and topography of free-standing chemically modified graphene
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The mechanical, electrical and chemical properties of chemically modified graphene (CMG) are intrinsically linked to its structure. Here we report on our study of the topographic structure of free-standing CMG using atomic force microscopy and electron diffraction. We find that, unlike graphene, suspended sheets of CMG are corrugated and distorted on nanometre length scales. AFM reveals not only long range (100 nm) distortions induced by the support, as previously observed for graphene, but also short-range corrugations with length scales down to the resolution limit of 10 nm. These corrugations are static not dynamic, and are significantly diminished on CMG supported on atomically smooth substrates. Evidence for even shorter range distortions, down to a few nanometres or less, is found by electron diffraction of suspended CMG. Comparison of the experimental data with simulations reveals that the mean atomic displacement from the nominal lattice position is of order 10% of the carbon-carbon bond length. Taken together, these results suggest a complex structure for chemically modified graphene where heterogeneous functionalisation creates local strain and distortion.
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The textbook thermophoretic force which acts on a body in a fluid is proportional to the local temperature gradient. The same is expected to hold for the macroscopic drift behavior of a diffusive cluster or molecule physisorbed on a solid surface. The question we explore here is whether that is still valid on a 2D membrane such as graphene at short sheet length. By means of a non-equilibrium molecular dynamics study of a test system -- a gold nanocluster adsorbed on free-standing graphene clamped between two temperatures $Delta T$ apart -- we find a phoretic force which for submicron sheet lengths is parallel to, but basically independent of, the local gradient magnitude. This identifies a thermophoretic regime that is ballistic rather than diffusive, persisting up to and beyond a hundred nanometer sheet length. Analysis shows that the phoretic force is due to the flexural phonons, whose flow is known to be ballistic and distance-independent up to relatively long mean-free paths. Yet, ordinary harmonic phonons should only carry crystal momentum and, while impinging on the cluster, should not be able to impress real momentum. We show that graphene, and other membrane-like monolayers, support a specific anharmonic connection between the flexural corrugation and longitudinal phonons whose fast escape leaves behind a 2D-projected mass density increase endowing the flexural phonons, as they move with their group velocity, with real momentum, part of which is transmitted to the adsorbate through scattering. The resulting distance-independent ballistic thermophoretic force is not unlikely to possess practical applications.
An acoustic plasmon is predicted to occur, in addition to the conventional two-dimensional (2D) plasmon, as the collective motion of a system of two types of electronic carriers coexisting in the very same 2D band of extrinsic (doped or gated) graphene. The origin of this novel mode resides in the strong anisotropy that is present in the graphene band structure near the Dirac point. This anisotropy allows for the coexistence of carriers moving with two distinct Fermi velocities along the Gamma-K direction, which leads to two modes of collective oscillation: one mode in which the two types of electrons oscillate in phase with one another [this is the conventional 2D graphene plasmon, which at long wavelengths (q->0) has the same dispersion, q^1/2, as the conventional 2D plasmon of a 2D free electron gas], and the other mode found here corresponding to a low-frequency acoustic oscillation [whose energy exhibits at long wavelengths a linear dependence on the 2D wavenumber q] in which the two types of electrons oscillate out of phase. If this prediction is confirmed experimentally, it will represent the first realization of acoustic plasmons originated in the collective motion of a system of two types of carriers coexisting within the very same band.
Chemical functionalization of graphene modifies the local electron density of the carbon atoms and hence electron transport. Measuring these changes allows for a closer understanding of the chemical interaction and the influence of functionalization on the graphene lattice. However, not only chemistry, in this case diazonium chemistry, has an effect on the electron transport. Latter is also influenced by defects and dopants resulting from different processing steps. Here, we show that solvents used in the chemical reaction process change the transport properties. In more detail, the investigated combination of isopropanol and heating treatment reduces the doping concentration and significantly increases the mobility of graphene. Furthermore, the isopropanol treatment alone increases the concentration of dopants and introduces an asymmetry between electron and hole transport which might be difficult to distinguish from the effect of functionalization. The results shown in this work demand a closer look on the influence of solvents used for chemical modification in order to understand their influence.
One of the most exciting phenomena observed in crystalline disordered membranes, including a suspended graphene, is rippling, i.e. a formation of static flexural deformations. Despite an active research, it still remains unclear whether the rippled phase exists in the thermodynamic limit, or it is destroyed by thermal fluctuations. We demonstrate that a sufficiently strong short-range disorder stabilizes ripples, whereas in the case of a weak disorder the thermal flexural fluctuations dominate in the thermodynamic limit. The phase diagram of the disordered suspended graphene contains two separatrices: the crumpling transition line dividing the flat and crumpled phases and the rippling transition line demarking the rippled and clean phases. At the intersection of the separatrices there is the unstable, multicritical point which splits up all four phases. Most remarkably, rippled and clean flat phases are described by a single stable fixed point which belongs to the rippling transition line. Coexistence of two flat phases in the single point is possible due to non-analiticity in corresponding renormalization group equations and reflects non-commutativity of limits of vanishing thermal and rippling fluctuations.
We investigate the morphology of quasi-free-standing monolayer graphene (QFMLG) formed at several temperatures by hydrogen intercalation and discuss its relationship with transport properties. Features corresponding to incomplete hydrogen intercalation at the graphene-substrate interface are observed by scanning tunneling microscopy on QFMLG formed at 600 and 800{deg}C. They contribute to carrier scattering as charged impurities. Voids in the SiC substrate and wrinkling of graphene appear at 1000{deg}C, and they decrease the carrier mobility significantly.
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