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Register a new userBallistic thermophoresis of adsorbates on free-standing graphene
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Added by
Emanuele Panizon Dr
Publication date
2017
fields
Physics
and research's language is
English
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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.
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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.
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.
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 magnetotransport properties of quasi-free standing epitaxial graphene bilayer on SiC, grown by atmospheric pressure graphitization in Ar, followed by H$_2$ intercalation. At the charge neutrality point the longitudinal resistance shows an insulating behavior, which follows a temperature dependence consistent with variable range hopping transport in a gapped state. In a perpendicular magnetic field, we observe quantum Hall states (QHSs) both at filling factors ($ u$) multiple of four ($ u=4, 8, 12$), as well as broken valley symmetry QHSs at $ u=0$ and $ u=6$. These results unambiguously show that the quasi-free standing graphene bilayer grown on the Si-face of SiC exhibits Bernal stacking.
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